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Carbonylation of olefins is carried out in the presence of a hydroxylic compound, carbon monoxide and a catalyst system comprising an organic phosphine liganded palladium compound and a perfluorosulfonic acid.
1. In an improved catalytic carbonylation process for preparing acids and esters by reacting an olefinically unsaturated compound, carbon monoxide and a hydroxylic compound, at about 50� to about 150� C., in the presence of a catalyst comprising an organic phosphine liganded palladium compound and an acid, wherein the improvement comprises using a perfluorosulfonic acid as the acid.
2. Process of claim 1 wherein the olefinically unsaturated compounds are nonconjugated hydrocarbons and contain 2 to 30 carbon atoms including a terminal olefinic group and the hydroxylic compound is water or a primary or secondary alcohol which contains 1 to 10 carbon atoms and 1 to 4 hydroxyl groups.
3. Process of claim 2 wherein the palladium is added to the reaction mixture as supported palladium, a tetrakis(trialkylphosphine)- or tetrakis(triarylphosphine) palladium compound, a palladium salt of a perfluorosulfonic acid, an arylphosphine liganded palladium salt of a perfluorosulfonic acid, or a palladium salt of a perfluorosulfonic acid polymer.
4. Process of claim 2 wherein the organic phosphine is a trialkylphosphine, a triarylphosphine, or an alkylarylphosphine.
5. Process of claim 2 wherein the organic phosphine ligand is triphenylphosphine, tri-p-tolylphosphine, tri-m-tolylphosphine, ethyldiphenylphosphine, methyldiphenylphosphine, propyldiphenylphosphine or 1,6-hexamethylenebis(diphenylphosphine).
6. Process of claim 2 wherein the perfluorosulfonic acid is trifluoromethanesulfonic acid, pentafluoroethanesulfonic acid, nonafluorobutanesulfonic acid, perfluorooctanesulfonic acid or a perfluorosulfonic acid polymer.
7. Process of claim 2 wherein the acid is trifluoromethanesulfonic acid.
8. Process of claim 2 wherein the acid is perfluorooctanesulfonic acid.
9. Process of claim 2 wherein the acid is a perfluorosulfonic acid polymer.
10. Process of claim 9 wherein the perfluorosulfonic acid polymer has a number average molecular weight of at least 5,000 and an equivalent weight of 500 to 20,000.
11. Process of claim 10 wherein the molar ratio of phosphorus to palladium is at least 4 to 1; the molar ratio of olefinically unsaturated compound to palladium is about 100:1 to 5,000:1; the molar ratio of acid to palladium is about 1:1 to 50:1; the partial pressure of carbon monoxide is about 0.1 to about 25 MPa; and the amount of hydroxylic compound is at least the amount stoichiometrically required to complete the reaction.
12. Process of claim 11 wherein the olefinically unsaturated compound is propylene and the hydroxylic compound is methanol.
13. Process of claim 12 wherein the palladium is added to the reaction mixture as a salt of a perfluorosulfonic acid polymer and the orgnic phosphine is triphenylphosphine.
14. Process of claim 13 wherein the perfluorosulfonic acid polymer has an equivalent weight of about 900 to about 2000 and contains less than 5 weight percent of hydrogen, chlorine and carboxyl groups, the molar ratio of olefin to palladium is 400:1 to 3000:1, and the temperature is 80� to 120� C.
This invention relates to palladium catalyzed carbonylation of olefinically unsaturated compounds in the presence of a perfluorosulfonic acid.
Carbonylation of olefins under mild conditions with minimum by-product formation based on palladium complex salts as catalysts, examples of which include palladium catalysts containing phosphines, phosphites, ammonia, amines, nitriles, and unsaturated hydrocarbons as ligands, is known.
Tsuji, Accounts Chem. Res. 2, 144-152 (1969) reviews palladium catalyzed carbon-carbon bond formation, including such carbonylation reactions. Bittler, et al., Agnew. Chem. Internat. Edit., 7, 329-335 (1968) disclose carbonylation of olefins under mild conditions in the presence of complex palladium (II) compounds and observe the Pd(O) compounds are inactive in the absence of added hydrogen chloride.
Several references disclose that certain metal halides, when added to the reaction mixture, improve the yield of linear products relative to branched products. These include, e.g., Mrowca, U.S. Pat. No. 4,257,973; Mrowca, U.S. Pat. No. 3,859,319; Butter, U.S. Pat. No. 3,700,706; Knifton, U.S. Pat. No. 3,919,272; and Knifton, J. Org. Chem., 41, 2885-2890 (1976). Use of such halides may pose corrosion problems. Fenton, U.S. Pat. No. 3,641,074 discloses the use of hydrogen and/or limiting mineral acid content of the reaction medium to favor the formation of linear rather than branched products.
Kajimoto, et al., U.S. Pat. No. 3,723,486 disclose the use of a palladium complex containing dichlorobenzene.
Yamaguchi, et al., U.S. Pat. No. 3,839,378 disclose the use of a palladium complex containing iodine or bromine and the use of hydrogen gas.
Cavinato et al., J. Mol. Catalysis, 10, 161-170 (1981), discuss effects of solvents on the hydrocarboalkoxylation of propylene with a palladium complex catalyst.
Hara, U.S. Pat. No. 3,793,369 discloses that it is desirable to employ a palladium complex with an aromatic tertiary phosphine, the molar ratio of the phosphine to palladium being 4:1 to 20:1.
von Kutepow, et al., U.S. Pat. No. 3,501,518, disclose carbonylation of olefins in the presence of metallic palladium or a palladium chalcogenide, a strong or medium strength acid (dissociation constant K>10-4) and an organic phosphine or nitrile. Sulfuric acid, perchloric acid, phosphoric acid and hydrogen halides are disclosed as useful acids. von Kutepow, et al., U.S. Pat. No. 3,437,676 disclose carbonylation of olefins in the presence of a complex palladium salt, e.g., bis(triphenylphosphine) palladium dichloride. The reaction may be carried out in the presence of an organic or inorganic acid such as sulfuric acid, phosphoric acid, boric acid, acetic acid, propionic acid, other carboxylic acids and hydrogen halides.
It is also known that carbonylation of olefins can proceed in the absence of a metal catalyst if a high concentration of a strong acid is employed. For example, Booth, et al., J. Chem. Soc. Perkin I. 2441-2446 (1979) and Norrell, U.S. Pat. No. 3,965,132 disclose improved yields when trifluoromethanesulfonic acid is employed instead of sulfuric acid.
It is an object of this invention to provide a process for carbonylation of olefins which process does not employ corrosive halides and which provides an increase in reaction rate in comparison with that achieved using known strong acids such as sulfuric acid.
For further comprehension of the invention, and of the objects and advantages thereof, reference may be made to the following further description and to the appended claims in which the level features of the invention are particularly set forth.
The invention resides in a process for the carbonylation of olefinically unsaturated compounds in which process the compounds are contacted and reacted with carbon monoxide and a hydroxylic compound in the presence of a catalytic amount of a catalyst system comprising an organic phosphine liganded palladium compound and a perfluorosulfonic acid at about 50� to about 150� C. for a time sufficient to effect reaction.
The carbonylation reaction is applicable to a wide variety of olefinically unsaturated compounds, including compounds with more than one ethylenic group and substituted compounds. At least two substituents of the olefinic group should be hydrogen, and the olefinic group should not be conjugated with other aliphatic unsaturated groups. Substituents which do not interfere with the carbonylation reaction include, e.g., aryl, alkoxy, alkoxycarbonyl, carboxyl, cyano, acyl and aroyl. Halo-substituted compounds may be employed provided that the halo- substituents are at least two carbon atoms removed from the olefinic double bond. Preferably the unsaturated compounds contain from 2 to 30 carbon atoms. Hydrocarbons with terminal olefinic groups are preferred.
Olefinically unsaturated compounds which may be carbonylated include, e.g., ethylene, propylene, butenes, pentenes, hexenes, octenes, decenes, tetradecenes, octadecenes, docosenes, 1,5-hexadiene, 1,9-decadiene, 4-vinylcyclohexene, methyl 10-undecenoate, 10-undecenoic acid, 10-undecene-1-ol, 5-hexene-2-one, 5-hexenenitrile and trans-1,4,9-decatriene.
Hydroxylic compounds which can be employed in the practice of this invention include water and primary and secondary alcohols which contain 1 to 4 hydroxyl groups, preferably 1, and which preferably contain from 1 to 10 carbon atoms. When an alcohol is employed in the carbonylation process, the product is an ester. When water is employed as the hydroxylic compound, a carboxylic acid is obtained as the carbonylation product. Particularly preferred hydroxylic compounds are saturated, aliphatic, monohydric primary and secondary alcohols which contain from 1 to 10 carbon atoms. Useful alcohols include, e.g., methanol, ethanol, propanol-1, propanol-2, butanol-1, pentanol-1, hexanol-1, β-methoxyethanol, benzyl alcohol, and neopentyl alcohol. It is preferred to employ alcohol or water in an amount stoichiometrically required to complete the reaction. Excess alcohol may be employed in the carbonylation process as a solvent.
The catalyst system comprises a zerovalent or divalent palladium compound, an organic phosphine ligand and a perfluorosulfonic acid. Palladium can be added to the reaction mixture in a variety of forms including, e.g., supported palladium such as palladium on carbon or silica, tetrakis(trialkylphosphine)- and tetrakis(triarylphosphine)palladium (0) compounds, palladium salts of perfluorosulfonic acids such as the palladium salts of trifluoromethanesulfonic acid and of perfluorooctanesulfonic acid, aryl-phosphine liganded palladium salts of perfluorosulfonic acids and, preferably, palladium salts of perfluorosulfonic acid polymers.
In general, the palladium catalyst is employed in a molar ratio of olefinically unsaturated compound to palladium of about 100:1 to about 5000:1, preferably about 400:1 to about 3000:1. Larger ratios may provide too little catalyst to achieve rate enhancement, and smaller ratios are uneconomical with regard to palladium.
Use of perfluorosulfonic acids with organic phosphine liganded palladium compounds has been observed to result in an increase in the rate of reaction in comparison to reactions carried out using sulfuric acid. Useful organic phosphine ligands include, e.g., trialkylphosphines, triarylphosphines such as triphenylphosphine, tri-p-tolylphosphine and tri-m-tolylphosphine; and alkylarylphosphines such as ethyldiphenylphosphine, methyldipheylphosphine, propyldiphenylphosphine, and 1,6-hexamethylenebis(diphenylphosphine). In a small number of experimental reactions, it was observed that the reaction did not proceed satisfactorily when certain alkylarylphosphines, namely, 1,2-dimethylenebis(diphenylphosphine) and 1,4-tetramethylenebis(diphenylphosphine), were used. It is believed that this was due to intramolecular cyclization. The triarylphosphines, especially triphenylphosphine, are preferred.
Excess amounts of phosphine ligand over that required to form a complex with the palladium compound are preferred to stabilize the catalyst complex. A molar ratio of phosphorus to palladium of at least about 4:1 is especially preferred.
Perfluorosulfonic acids which can be employed include, e.g., trifluoromethanesulfonic acid, pentafluoroethanesulfonic acid, nonafluorobutanesulfonic acid, perfluorooctanesulfonic acid, and perfluorosulfonic acid polymers. Preferred are perfluorosulfonic acid polymers which have a number average molecular weight of at least about 5000. The polymer should contain a sufficient number of sulfonic acid groups to give an equivalent weight of about 500 to about 20,000, preferably about 900 to about 2000. Although the polymer backbone will largely comprise perfluorinated carbon atoms, it is not necessary that all other atoms be excluded. For example, ether oxygen may be present in the backbone or in the side chains of the polymer. Other atoms or groups such as hydrogen, chlorine and carboxyl groups may be present in limited amounts without significantly affecting the stability or operability of the polymer under the process conditions. It is preferred that the polymer contain no greater than about 5 weight percent total of such other atoms or groups. The perfluorosulfonic acid may be employed directly as an additive or as a preformed palladium salt of the acid.
Typically, the perfluorosulfonic acid is employed in a molar ratio of acid to palladium of about 1:1 to 50:1, preferably about 4:1 to 25:1.
Although a solvent is not required for the carbonylation reaction, it may be advantageous to employ one, particularly when higher molecular weight olefinically unsaturated compounds are employed as substrates. Alternatively, as noted above, an excess quantity of an alcohol reactant may be employed as a solvent. If a solvent is used, an important factor to be considered in the selection of one suitable for a particular carbonylation reaction, is the boiling point difference between the solvent and the carbonylated product. The boiling point difference should be such as to enable efficient separation of the solvent and product by simple distillation. Suitable solvents include aromatic hydrocarbons such as benzene, toluene and the xylenes, chlorinated aromatic hydrocarbons such as o-dichlorobenzene, and miscellaneous solvents such as acetonitrile and tetramethylenesulfone.
The carbonylation reaction of this invention is effected by heating the olefinically unsaturated compound, the hydroxylic compound, the palladium catalyst system, and the perfluorosulfonic acid in an atmosphere of carbon monoxide at a temperature of about 50� to about 150� C., preferably about 80 to about 120� C. Carbon monoxide pressures of about 0.1 to about 25 MPa or more can be used although it is preferred to employ pressures in the range of about 5 to about 15 MPa. The reaction may be run for as long as about 24 hours, but 0.5 to 5 hour reaction periods generally suffice and are preferred.
The process of the invention can be readily carried out using well-known chemical engineering practices which include continuous, semi-continuous and batch operations.
The type of reactor used in this invention is not critical as long as it is able to withstand the temperatures and pressures involved. Pressure vessels of high tensile steel are typically used, either lined or unlined. Suitable reactor liners include Hastelloy� metals, stainless steel, silver, copper, tantalum, glass and glazed ceramics.
The reaction is carried out by charging the olefin, if liquid or solid, the hydroxylic compound, the catalyst system and any solvent into a suitable pressure-resistant vessel. For laboratory work, a shaker or rocker system is convenient for agitating the reactants and effecting intimate contact of the reactants. The charged reactor is closed, chilled in dry ice, evacuated and placed in a shaker or rocker. The olefinically unsaturated compound, if gaseous, is then added and the system is connected to a supply of carbon monoxide. Sufficient carbon monoxide is added to give the desired pressure at the chosen reaction temperature.
The system is then heated under agitation until reaction is complete. As the reaction proceeds, more carbon monoxide may be added periodically to maintain the pressure in the desired range. The course of the reaction is readily followed by observation of the drop in pressure. The product or products can be removed from the reaction mixture by conventional methods of isolation such as distillation.
The following are illustrative examples of the invention in which all parts and percentages are by mol, and all degrees are Celsius unless otherwise noted. Conversions were calculated by the equation: Conversion=mols ester/mols olefinically unsaturated compound charged. The reported relative amounts of iso-ester (iso) are mols isobutyrate/(mols isobutyrate+mols n-butyrate).
The amounts of total ester and iso- ester obtained were determined by a standard gas chromatographic procedure using a 10'�1/8" column of 10% SE-30 on 80/100 mesh diatomaceous earth. A temperature program of 110� (2 min) to 220� was utilized with a helium flow of about 30 ml/min. Response factors referenced against toluene (internal std) were employed to calculate the mols of products.
In the general carbonylation procedure employed, a 330 mL stainless steel shaker tube was flushed with nitrogen and charged with the palladium compounds, the arylphosphine, and the alcohol which contained the perfluorosulfonic acid. The tube was cooled to -78� C., and the specified quantity of olefinically unsaturated hydrocarbon was condensed into the tube. The tube was closed, connected to a pressure cell unless otherwise noted, and heated to the specific reaction temperature. Carbon monoxide was then added to the tube until the desired pressure was reached. The carbonylation reaction was carried out for 1 hr, and a pressure vs. time curve was recorded. The tube was cooled to room temperature, the reaction mixture was filtered to remove any solids, and the liquid product mixture was analyzed.
The pressure vs. time curve was used to measure the initial rate of carbonylation at low conversion of olefin. The initial rate was normalized for the number of moles of palladium initially charged. The units employed to define the initial turnover rate are mol ester/mol Pd/hr.
In this example, carbonylation of propylene was carried out at 105� and 13.8 MPa carbon monoxide pressure for 2 hrs by the general procedure except that a pressure cell was not employed. The tube was charged as follows:
1.0 mol propylene
1.5 mols methanol
11.5 mmols triphenylphosphine
1.29 mmols [(C6 H5)3 P]4 Pd
2.25 mmols CF3 SO3 H.
As the reaction proceeded, additional carbon monoxide was added in increments to maintain the pressure at 13.8 MPa. No pressure drop occurred after the first hour of reaction. Conversion to product ester was 53.4% with a 30.8% iso content; 410 mol ester/mol Pd/hr.
In these examples, carbonylation of propylene was carried out at 100� and 13.8 MPa carbon monoxide pressure by the general procedure, as follows:
0.33 mol propylene
0.50 mol methanol
0.43 mmol [(C6 H5)3 P]4 Pd
4.96 mmols triphenylphosphine.
The results, summarized in Table I, show an increased rate of reaction with added perfluorosulfonic acid compared with an equivalent protonic amount of the dibasic acid, sulfuric acid.
TABLE I______________________________________Homogeneous Catalyst Acid, Conversion Iso, Mol ester/Example mol � 103 % % mol Pd/hr______________________________________2 FC-95,.sup.(1) 37.5 28.9 678 2.263 CF3 SO3 H, 47.4 28.9 828 2.274 CF3 SO3 H, 92.5 32.7 1262 9.07Control A H2 SO4, 22.2 25.5 382 1.12______________________________________ .sup.(1) FC-95 is C8 F17 SO3 H
In these examples, carbonylation of propylene was carried out at 13.8 MPa carbon monoxide pressure using a heterogeneous palladium catalyst by the general procedure, as follows:
0.33 mol propylene, unless otherwise noted
0.50 mol methanol
5 wt. % palladium-on-carbon; 0.43 mmol Pd
6.68 mmol triphenylphosphine.
The results, summarized in Table II, show an increased rate of reaction with added perfluorosulfonic acid compared with an equivalent protonic amount of the dibasic acid, sulfuric acid.
TABLE II______________________________________Ex- Acid, Conversion Iso, Mol ester/ample mol � 103 Temp % % mol Pd/hr______________________________________5 FC-95, 100 48.4 28.9 805 2.266 CF3 SO3 H, 100 54.8 28.6 1498 2.297.sup.(1) CF3 SO3 H, 100 37.5 29.7 845 2.278 CF3 SO3 H, 80 21.9 25.0 295 2.27Con- H2 SO4 100 26.2 27.3 349trol B 1.14______________________________________ .sup.(1) 0.67 mol propylene was used
Carbonylation of propylene was carried out at 100� and 13.8 MPa carbon monoxide pressure by the general procedure, as follows:
0.33 mol propylene
0.50 mol methanol
0.43 mmol [(C6 H5)3 P]4 Pd
4.96 mmol triphenylphosphine
PFIEP; 2.26 milliequivalents sulfonic acid group.
PFIEP is a Du Pont Nafion� perfluorosulfonic acid polymer of equivalent weight 1100 as determined by titration of the sulfonic acid groups.
Carbonylation gave 23.1% conversion to reaction product which contained 27.6% iso ester product. The mol ester/mol Pd/hr was 719.
These examples illustrate the carbonylation reaction in which a palladium salt of a perfluorosulfonic acid polymer is employed as a catalyst. The catalyst was prepared by reaction of PFIEP (22.8 g; 20.1 milliequivalents sulfonic acid groups) with 2.32 g (9.04 mmol Pd) of Pd(NO3)2.XH2 O (41.3 wt. % Pd) at 60� for 1 hr with stirring. The reaction mixture was allowed to stand at room temperature for 11 days. The resin was separated by filtration, and the aqueous filtrate was titrated with 0.1 N sodium hydroxide for liberated nitric acid; 16.3 mmol. The resin was dried at 110� for 8 hrs under nitrogen to give 23.4 g of reddish-black product having 3.25 wt. % palladium (Catalyst A). Analogous procedures were employed to prepare resins which contained 1.34 wt. % palladium (Catalyst B) and 1.55 wt. % palladium (Catalyst C).
Carbonylation was carried out at 13.8 MPa carbon monoxide pressure by the general procedure, as follows:
0.33 mol propylene, unless otherwise noted.
0.50 mol methanol.
The results are summarized in Table III.
TABLE III______________________________________ Con- Mol ver- ester/Ex- Pd Catalyst, (C6 H5)3 P, Temp, sion Iso molample mol � 103 Pd mol � 103 �C. % % Pd/hr______________________________________10 B, 0.13 6.68 100 22.2 26.9 180711 C, 0.49 20.0 100 42.0 26.8 81712 A, 0.34 6.68 100 16.8 26.3 29413.sup.(1) A, 0.34 6.68 100 12.0 27.1 16914 C, 0.16 6.68 140 3.5 24.4 47715 A, 0.43 6.68 130 15.8 25.9 336______________________________________ .sup.(1) 0.17 mol propylene was used
In these examples, carbonylation of a designated olefin was carried out at 100� and 13.8 MPa carbon monoxide pressure by the general procedure using in each example a homogeneous catalyst obtained from 0.43 mmol [(C6 H5)3 P]4 Pd and 4.96 mmols triphenylphosphine. The results, summarized in Table IV, show an increased rate of reaction with added trifluoromethanesulfonic acid compared with an equivalent protonic amount of the diabasic acid, sulfuric acid.
In these examples the effect of carbon monoxide pressure on propylene carbonylation was studied at 100� using the general procedure, as follows:
0.33 mol propylene
0.50 mol methanol
5 wt. % palladium-on-carbon; 0.43 mmol Pd
6.68 mmol triphenylphosphine
PFIEP; 2.26 milliequivalents sulfonic acid groups.
The results are summarized in Table V.
TABLE IV______________________________________ Mol es-Hydrox- Con- ter/ylic ver- molCompound, Acid, Olefin, sion Iso, Pd/Ex. mols mols � 103 mols % % hr______________________________________16 Ethanol CF3 SO3 H, Propylene, 53.9 25.6 6660.34 2.27 0.3317 Methanol, CF3 SO3 H, Cis-2- 22.4 39.9.sup.(1) 5410.50 2.29 Butene, 0.3418 Methanol, CF3 SO3 H, Cis-2- 26.5 38.9.sup.(1) 5520.50 2.29 Butene, 0.3419 Water.sup.(2) CF3 SO3 H, Propylene, 1.1 24.3 230.50 2.27 0.33-- -- -- -- -- --* Ethanol, H2 SO4, Propylene, 17.4 26.4 2400.34 1.12 0.33** Methanol, H2 SO4, Cis-2- 6.9 45.6.sup.(1) 1930.50 1.12 Butene, 0.34*** Water.sup.(2) H2 SO4, Propylene, 0 -- --0.50 1.12 0.33______________________________________ .sup.(1) The products obtained were methyl 2methylbutyrate (iso) and methyl valerate (n). Examples 17 and 18 are duplicate runs. .sup.(2) Tetramethylenesulfone, 15 ml, was added as a solvent. *Control C **Control D ***Control E
TABLE V______________________________________ CO Pressure Conversion, Iso, Mol esterExample (MPa) % % mol Pd/hr______________________________________20 6.9 28.4 29.0 25221 13.8 28.5 28.2 35322 20.7 16.4 27.8 250______________________________________
In these examples the bisphosphine ligand, (C6 H5)2 P(CH2)6 P(C6 H5)2, was employed. Carbonylation of propylene was carried out at 100� and 13.8 MPa carbon monoxide pressure by the general procedure, as follows:
0.33 mol propylene
0.50 mol methanol
3.3 mmol (C6 H5)2 P(CH2)6 P(C6 H5)2.
The results, summarized in Table VI, show an increased rate of reaction with an added perfluorosulfonic acid compared with an equivalent protonic amount of the dibasic acid, sulfuric acid.
TABLE VI______________________________________ Con- ver- Pd Catalyst, Acid, sion Iso, Mol ester/Example mol � 103 Pd mol � 103 % % mol Pd/hr______________________________________23 5 wt. % Pd/C; CF3 SO3 H, 7.7 16.9 128 0.43 2.2724 Ex. 12, -- 8.4 16.7 226 Cat. A; 0.43-- -- -- -- -- --Control 5 wt. % Pd/C; H2 SO4, 5.2 16.9 72F 0.43 1.12______________________________________
In this example, carbonylation of propylene was carried out at 100� and 13.8 MPa carbon monoxide pressure for 2 hrs by the general procedure except that a pressure cell was not employed. The tube was charged as follows:
1.0 mol propylene
1.5 mol methanol
15.3 mmols triphenylphosphine
0.75 mmol Pd as the palladium salt
(3.95 wt. % Pd) of PFIEP, prepared by the procedure described in Examples 10-15.
As the reaction proceeded, additional carbon monoxide was added in increments to maintain the pressure at 13.8 MPa. No pressure drop occurred after the first 30 min of the reaction. Conversion to product ester was 22.3% with a 29.3% iso content; 599 mol ester/mol Pd/hr.
The best mode contemplated by the applicant for carrying out his invention is described by Examples 3, 6, 9 and 10 which show large increases in reaction rates.
Esters are a well-known class of useful organic compounds. Many esters are useful as solvents, and as plasticizers for polymers. Some esters are useful in perfumes, essences, and flavoring agents. Diesters and additionally useful for making polymers, such as polyesters and polyamides.
Carboxylic acids which can be made by the process of this invention are also well knwon to have a variety of uses. Higher molecular weight acids can be used in detergent compositions. Many low molecular weight acids, and particularly salts thereof, are useful as preservatives, as buffering agents, and as solvents. Acids are also extremely important intermediates for the manufacture of ketones, amides, esters, nitriles and many other organic compounds.
While the preferred embodiments of the invention are disclosed by the above, it is to be understood that the invention is not limited to the precise constructions herein disclosed and that the right to all modifications coming within the scope of the following claims is reserved.
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Cheap and Easy Crafts
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DIY Vintage Candles
By: Lina for Fancy Frugal Life
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Need some easy homemade gift ideas? Give these DIY Vintage Candles a try. Working with burlap is a breeze, and it can really match any decor style. Make these candles for a friend, a wedding, or just for yourself!
- Online stamp (these were from The Graphics Fairy)
- Printable linen fabric
- Burlap fabric
- Scissors
- Hot glue gun
- Pillar candles
- Paste your stamps of choice into a Word document and print them out on the printable fabric.
- Measure around the candle to see how long your fabric strips need to be, then cut out the linen strip. Cut the burlap strip a little bigger than the linen strip.
- Hot glue the strips to the candles. Add ribbons if you'd like!
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Article | October 31, 1997
Standardizing Canadian regs
Beset by an expanding array of provincial and municipal solid waste collection and disposal regulations, the Packaging Assn. of Canada is calling for legislation that standardizes requirements among all the provinces.
The group also called for provincial and municipal governments to share more of the costs of waste management.
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A Webcomic
Hey gang, I'm off to Canada for Christmas, to visit relatives, and drink that sweet, sweet maple syrup.
Chapter 19 will be wrapping up this week. We're going to take a week off for the holidays, (with art of course!) and start Chapter 20 on January 5th.
My friend Cristina is running a Kickstarter for her comic, Ball & Chain, be sure to check it out:


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Synonyms for overdraftˈoʊ vərˌdræft, -ˌdrɑft
This thesaurus page is about all possible synonyms and similiar words for the term overdraft
Princeton's WordNet
a draft in excess of the credit balance
Find a translation for the overdraft synonym in other languages:
Select another language:
Discuss these overdraft synonyms with the community:
Use the citation below to add these synonyms to your bibliography:
"overdraft." Synonyms.net. STANDS4 LLC, 2014. Web. 21 Dec. 2014. <http://www.synonyms.net/synonym/overdraft>.


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Israel Hernandez: One Year Later, Still No Answers
By Michael E. Miller
Five Reasons Miami Heat Fans Deserve Respect
By Ryan Yousefi
FL Doctors Comes Out Against Medical Marijuana
By Kyle Munzenrieder
All Aboard Florida New Images of Miami Station
By Sabrina Rodriguez
Miami VA Director Responds To Neglect Scandal
By Michael E. Miller
Miami artist AholSniffsGlue Sues American Eagle
By Carlos Suarez De Jesus
2 Live Crew's Legal Fight Is Still Vital 25 Years Later
By Luther Campbell
Report: 90 Percent of Condo Buyers Are Foreigners
By Kyle Munzenrieder
Hello, Kitty: My relationship with my mom has been strained ever since I dropped out of college to pursue a career selling jeans at the Gap. But not long ago, I lost my job, and she offered up her spare bedroom. I'm guessing that it was simply lip service since she now tells me to get out daily. And not with words. In the worst way. She and her boyfriend (who's 12 years her senior) have sex all the time and run around naked when they're not joined at the hip. Prior to my moving in, their touchy-feeliness told me that they had a healthy sex life, but I never knew how healthy. When I wake up in the morning, I hear them humping. When I go out to get some Subway around noon, they're getting freaky in the dining room; and when I get back, they're lounging around the kitchen in the nude! I know that my mom can do what she likes in her house, but I'd like for her to respect that I'm there. I know I'm her daughter and only 27, but how can I ask this grown woman to cut back on the fuckery while I'm around?
Troma Ties
Hey, Troma: You can't tell her to stop. What you can tell her is, "Mom, I found a job. I'm moving out." It's too bad the Gap downsized and you had to return to the womb, but that's your problem, not your mom's. If she wants to dick around at 10 a.m., 4 p.m., and half past midnight, she has the right. If you had been enterprising enough to find a man or friends to shack up with when times got rough, you wouldn't have to smell tu madre's badussy mingling with the scent of the onions from your $5 foot long. I don't necessarily agree that your mom is using sex as a weapon to convince you to leave – this is probably how she was living before you moved back in. She may have considered easing up but decided against it. In her house, she rules. What you can do is get a life or a job, whatever you can do to not be in the house so often. Though she may seem unfazed by the sight of you while her old man is sticking her, it's probably making her uncomfortable too. However, if they stopped doing it so often, the dynamic of their relationship could change, resulting in a breakup. All your fault. Get a job, move in with friends, leave Mom to her fuckery. Meow.
Got a question? Email firstname.lastname@example.com, or visit blogs.miaminewtimes.com/riptide/magic_city_kitty
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Vegan Dumplings at Rickshaw; Grand Street Gourmet Shutters
Brooklyn Heights feels the reverberations of an accused-con-man restaurant manager, and R&L restaurant sees another setback, in today's neighborhood food news.
Skip to content, or skip to search.
Skip to content, or skip to search.
Brooklyn Heights feels the reverberations of an accused-con-man restaurant manager, and R&L restaurant sees another setback, in today's neighborhood food news.
Pump it up, until you can feel it...
So, will folks start going there now?
The latest clubhouse-themed meatpacking-district lounge is owned by an actor and a baseball player.
But who will get the restaurant's coveted liquor license?
One month after taking over from Florent, R&L Restaurant is without booze, and without customers.
Ten varieties of gourmet popcorn!
Plus Ben & Jerry's new Elton John–inspired ice cream, a book about cannibalism, and more, in our morning news roundup.
Is Merkato 55 meant to be just a nightclub?
The twenty-year-old neighborhood standby closed this weekend.
The 'Top Chef winner' comes home to roost.
When you can't get a drag queen to show up to the party, a mime will do.
He got his start selling sunglasses in order to pick up girls.
But how long will Joanne Lucas stay in the restaurant business?
Also, Steve & Barry's closures are imminent, and Eva Mendes makes a suprisingly bold statement about the couture collections.
The scene last night.
Yesterday brought a new basement lounge. Today, a rooftop bar.
Like all hot spots these days, the lounge under Merkato 55 is accessed through a "private" door and a service hallway
Bijou lounge hides beneath Merkato 55, and Le Pain Quotidien mobilizes staff for its big opening in Tribeca, in our daily neighborhood roundup.
Florent ended its 23-year run early this morning with an intimate wrap party. 'New York''s David Amsden was there.


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Morningstar Farms has hot dogs again
Morningstar Farms has hot dogs again.
I got some about a month ago. They aren't quite as good as the old ones and you get less for more $$ and they are in a box in the frozen section by the other MSF products.
Just thought I'd mention it.
I definitely agree. The ones they used to sell in the shrink-wrapped hotdog package were much better. I was pretty disappointed. I don't care for Smartdogs or the Tofurkey brand ones either. :( I do like the Torfurkey brats as a substitute, but they always fall off my hotdog stick!
I heard that Field Roast hot dogs are good, but I can never find them, only the sausage types.
As for Tofurky, the one I like is the sliced hickory smoked kind...but that's just for a sandwich type wrap. I didn't care for smart dogs or tofurky dogs or any of the other ones I have tried. I think it was tofu pups instead of tofurky dogs, but they are probably very close to the same thing.
Try the VeggiePatch hot dogs. Best veggie dog I've ever had! Most Wal-Mart's have them, located in the same section with Morningstar. Their corndogs are pretty yummy too!!
I did try the veggie patch, but the garlic in them did me in. I have an allergy to garlic. I can eat something if it has tiny amounts in it, but only once in a great while. Most of the time, it tears up my stomach.
Also, the corndogs aren't low carb, unfortunately.
|All times are GMT -7. The time now is 10:05 PM.


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Post office reports record loss of $15.9B for year
WASHINGTON (AP) — The struggling U.S. Postal Service on Thursday reported an annual loss of a record $15.9 billion and forecast more red ink in 2013, capping a tumultuous year in which it was forced to default on billions in payments to avert bankruptcy.
The financial losses for the fiscal year ending Sept. 30 were more than triple the $5.1 billion loss in the previous year. Having reached its borrowing limit, the mail agency is operating with little cash on hand, putting it at risk in the event of an unexpectedly large downturn in the economy.
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Rebranding BP: Top 10 New BP Logo Ideas
That's probably enough from the department of subtlety. The No. 4 new BP logo idea edges to the more extreme end of response to the BP oil spill.
No. 4 really pushes the envelope in representing the bad, the ugly, and the downright violent impulses from otherwise good people that have been stewing in the Gulf and about the Gulf, from an "ass to kick" to a "boot on BP's neck" to the more questionable end of the violent BP oil spill images.
Some of the BP failed methods for controlling the oil spill sounded downright violent, from the "top kill" to the "junk shot" to the "overshoot," yet they all demonstrated the high-tech efficiency of a slingshot or potato gun.
It's a little surprising, in a good way, that public anger over the BP oil spill has not turned more violent. There were reports of a protest in Los Angeles turning into a violent altercation between police and citizens in late May, but for the most part, the American public has behaved in a way that makes BP's behavior look even worse.President Obama has changed his tune during the oil spill, from telling Larry King that he wasn't the one who should be "yelling and screaming" to bypassing verbal attacks on his hunt for an "ass to kick." All in all, though, while there has been lots of angry testimony in the Gulf region and the inevitable boycotting of BP gas stations, America has remained Beyond Paroxysm. It's a fine line between good behavior and a feeling of helplessness, though. With more recent attacks being laid at the unhinged door of BP centered on failure to pay claims to those economically devastated by the oil spill, the quiet can seem ominous, too, and the prospect of an unhinged Gulf coast population not hard to imagine.
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Here we are now, one more time, on the Senate floor to retell the story of one of the most tragic episodes in the history of the Armenian people or any people. It is clearly a tragedy that has scarred every Armenian family that is alive today.
We do this to remember the suffering of the Armenian people in order to ensure the accuracy of the historical record and to challenge those who would like to believe that this act of genocide never occurred.
While we consider this somber issue, I want to particularly commend the minority leader [Senator Dole] for his outstanding leadership in moving ahead with this resolution, despite strong pressure from a number of directions to drop its consideration or water down its pertinent language. So I am pleased to join him in signing the cloture motion [to try and stop Senator Byrd's filibuster]. Let us go ahead and vote; I think this is crucial.
Despite overwhelming evidence of the death of between 1 and 2 million Armenians the world has still not acknowledged the suffering inflicted on Armenians by the Turkish Ottoman Empire 75 years ago. With the passage of this resolution, humanity will be more keenly aware of the devastation inflicted on the Armenian people.
In the waning days of the Ottoman Empire, Turkish rulers began to view the growing Armenian nationalist spirit as a threat to the control of their huge domain. Literally, hundreds of thousands of Armenian men, women and children were slaughtered or starved to death in vicious attempts to quell the Armenian drive for self-determination.
The scope of the inhumanity revealed itself on the night of April 14 [sic, this should be April 24], 1915, when Turkish police rounded up all of the Armenian intellectuals from their homes in Constantinople, effectively silencing the voice of a generation. Not long after, in a no less reprehensible fashion, Armenians serving in the Ottoman Army were disbanded and disarmed, removing any possible protection for the Armenian minority. Powerless and overwhelmed by the cruelty of their Ottoman captors, Armenians were deported from cities and towns throughout Turkey and Asia Minor. A majority of the deportees perished when forced on long death marches to the deserts of what is now Syria and Iraq.
The end of World War I brought a short period of relief for the surviving Armenians. In 1918, the ill-equipped Armenian Army, comprised of refugees and volunteers from abroad, arose and defeated invading Turkish forces. On May 28 of that year, having thwarted the designs of their invaders, Armenians triumphantly established an independent and sovereign state. Although Turkey and the Soviet Union pledged to respect the independence of the newly formed state, 1918 concluded with the tragically successful invasion of armies from both Turkey and the Bolshevik Soviet Union. Eastern Armenia subsequently was renamed the Armenian Soviet Socialist Republic, while Armenians under Turkish rule continued to face butchery at the hands of their former oppressors.
These deliberately perpetrated atrocities, which virtually eliminated the entire Armenian community of the Ottoman Empire, should forever be recalled as one of the most horrific acts of genocide ever perpetrated against an ethnic community anywhere.
Unfortunately many continue to deny the indisputable testimony provided by numerous observers and survivors. At the same time, I agree with the point that those on the other side have made. That is, while we stress the importance of establishing the factual accuracy of the genocide of the Armenian people, it is important to point out that this resolution is not directed against the present Turkish Government and it is not intended to harm the deep ties between the United States and Turkey.
The genocide of the Armenian people occurred long before the current Republic of Turkey was ever created.
But there is nothing that so clearly threatens our future than the refusal to recognize the mistakes of the past. Not to acknowledge the full extent of the suffering of the Armenian people is an offense, not only to the victims of that genocide, but also to those who have survived in the generations of Armenians that followed. A half-hearted position of the United States Government to the recognition of the Armenian genocide raises a question as to whether were are committed to the spirit of the recently ratified United Nations treaty against genocide.
I think we must align ourselves firmly on the side of truth and human rights and recognize clearly and forcefully and without ambiguity the suffering of the Armenian people.
I want to note as well that the Armenian Research and Publishing Center, the only one that we have affiliated with an American University, is located in my home state in Dearborn, MI. This is a very important center that has helped America and the world learn of the historic relationship between the Armenian and American peoples and will continue to help balance, with objective scholarship, the efforts of those who seek to alter history by denying the significance of the Armenian Genocide.
The large Armenian-American community in Michigansome 60,000 peoplehas made and continues to make a powerful and positive statement about the vitality of the Armenian people and the validity of their cause. Moreover, as a unified group around the world, Armenians have represented a powerful symbol against persecution and oppression. Their consistent pursuit of the truth has resulted in the resolution before the Senate today which would recognize and remember the genocide of 1915-1923.
Others today who spoke before me recalled the words of others; Ambassador Morgenthau, even that of Adolf Hitler. When it was suggested to Hitler that world public opinion would be hostile if he proceeded with his so-called solution to the Jewish problem he responded, "Who, after all, speaks of the annihilation of the Armenians?"
The world has proven Hitler wrong and we have remembered the crimes against the Jewish people. And it is imperative that we do no less for Armenians. Because ignorance of history is an invitation to repeat it. And I daresay the genocides that we have seen in the years past may be, in part, due to the fact that there was too little attention paid at the time, or since, to the Armenian genocide.
So it is through the passage of Senate Joint Resolution 212 that the Senate can assist Armenians in the United States and abroad in enlightening the world to the tragic act of genocide and in so doing assure that history does not repeat itself.
I think to those who suffered directly at that time and to those who are part of the bloodline that flows from that time forward to today, that we have an obligation to see that these facts are put out in to the clear light of day. Some may not like it. It may challenge some centers of power here or there.
I think it is very important that we get the historical record out here, that it be in the clear light of day, that we put the issue to a vote and put the Senate on record.


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Eddie Cooke Joins The Bank Of Hampton Roads As Vice President
VIRGINIA BEACH, Va., Dec. 20, 2012 (GLOBE NEWSWIRE) -- Hampton Roads Bankshares, Inc. (Nasdaq:HMPR) (the "Company"), the holding company for The Bank of Hampton Roads ("BHR") and Shore Bank, today announced that Joseph E. (Eddie) Cooke has joined BHR as a Vice President and commercial lender serving the Outer Banks, North Carolina market. Cooke will report to Chuck Parker, President, Outer Banks Market.
Douglas J. Glenn, President and Chief Executive Officer of the Company and Chief Executive Officer of BHR, said, "We welcome Eddie to our team. He brings three decades of experience in commercial and small business lending and other financial services. With the addition of Eddie, we continue our progress in building the premier community bank lending team in each of the regions we serve, providing a strong foundation for loan and deposit growth going forward."
Prior to joining BHR, Cooke served as Vice President/City Executive at Southern Bank and Trust Company in Kill Devil Hills, NC. From 1999 to 2005, he served as Assistant Vice President at Wachovia Bank, where he provided financial planning services for bank customers. From 1996 to 1999, Cooke served in sales and sales management positions with Coggin Insurance Agency, Inc. and Prudential Insurance and Financial Services. From 1982 to 1996, he served in a variety of positions with Centura Bank, most recently as Assistant Vice President and retail and commercial lender.Cooke earned a BA in Business Management and Economics from North Carolina State University. He currently serves as President of the Outer Banks Forum for the Lively Arts and an Outer Banks Chamber of Commerce Ambassador. Caution About Forward-Looking Statements Certain statements made in this press release may constitute "forward-looking statements" within the meaning of the Private Securities Litigation Reform Act of 1995. Forward-looking statements are statements that include projections, predictions, expectations, or beliefs about events or results or otherwise are not statements of historical facts, including prospective statements about the performance of the Company's personnel. Although the Company believes that its expectations with respect to such forward-looking statements are based upon reasonable assumptions within the bounds of its existing knowledge of its business and operations, there can be no assurance that actual results, performance or achievements of the Company will not differ materially from those expressed or implied by such forward-looking statements. Factors that could cause actual events or results to differ significantly from those described in the forward-looking statements include, but are not limited to those described in the cautionary language included under the headings "Risk Factors" and "Management's Discussion and Analysis of Financial Condition and Results of Operations" in the Company's Annual Report on Form 10-K for the fiscal year ended December 31, 2011, Quarterly Report on Form 10-Q for the quarter ended September 30, 2012 and other filings made with the SEC.
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Watch Ellen tease Jennifer Lawrence and the other nominees in her Oscars opening Monolouge!
Watch Ellen tease Jennifer Lawrence and the other nominees in her Oscars opening Monolouge!
It was a huge night at the 56th GRAMMY Awards for Macklemore & Ryan Lewis…not only did they sweep the rap categories and pick up 4 GRAMMY Awards, but their powerful performance of 'Same Love' will go down as one of the most iconic moments in GRAMMYs history!
We spoke to them backstage after the show and got their reaction!
Check video of all the performances from music's biggest night!
Zedd and Foxes picked up the GRAMMY Award for 'Best Dance Recording' for their song 'Clarity' during the pre telecast!
They stopped by backstage after picking up the award to give us their reaction!
One of the most fun things about awards shows is seeing where all your favourite artists are seated in the audience, and we've got a sneak peek at the seating chart for Sunday nights GRAMMY Awards!
While the rest of the world is talking about her, we're talking to her!
Watch as Adam Wylde sits down for an exclusive one-on-one interview with the most buzzed about singer on the planet…Miley Cyrus!
A month of incredible performances culminated last night at the Roundhouse in London, as Katy Perry took the stage for the finale of the iTunes Festival!
The month long iTunes Festival has seen some amazing performances from some of musics biggest stars, but there's not a star brighter than Justin Timberlake, who proved why he's the worlds best entertainer at his iTunes Festival gig on Sunday night!
The man of the moment, Robin Thicke, took the stage at the iTunes Festival on Tuesday night, and while Miley Cyrus was nowhere to be found, it didn't stop Thicke from delivering a memorable performance!
The Price Tag singer headlined Monday night of the iTunes Festival at the Roundhouse in London, with a wild a performance that worked the UK crowd in to a frenzy!


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My son is asked to repeat second grade, should I put him in a new school ?
My son who is in year 3, is an average student. The teacher asked us to put him in year 3 for one more year. We are okay with that, but am little concerned how he will digest it. How he will cope up, when all his friends move to a different class. I am thinking whether to put him at year 3 itself, in a new school ? Anyone else who has went through a similar situation, how did you manage ?In Topics: School and Academics, Motivation and achievement at school
Thank you
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Arizona's Top Election Official Goes Birther, Threatens To Keep Obama Off The Ballot
"Arizona's Top Election Official Goes Birther, Threatens To Keep Obama Off The Ballot"
Bennett is the latest Republican elected official to call into question Obama's place of birth in recent months. His comments were first flagged by the site White House Dossier:
BENNETT: First of all, I'm not playing to the birthers, I'm not a birther. I believe that the president was born in Hawaii, or at least I hope he was…Hawaii has a special provision in their law that allows other government officials from other states to request what's called a verification in lieu of a certified copy of a birth certificate. So I'm not asking for the certified copy of the birth certificate at all…I was frankly expecting that they would very quickly and very simply say 'yes.' Eight weeks later, they haven't said, I can't seem to get them to say yes.
In fact, Hawaii said "yes" over a year ago. Last April, Obama released a certified copy of his long form birth certificate to the public. And while that did nothing to quell the furor of birthers like Maricopa County, Arizona Sheriff Joe Arpaio, it more than meets Bennett's verification requirement.
And yet Bennett is insisting on still more costly and time-consuming work by the state of Hawaii to verify they have the original document on hand. The reason for his suspicion? Arpaio's sham investigation into the copy released by President Obama raised sufficient questions:
BENNETT: When Sheriff Joe Arpaio's posse released a press conference a few week ago, or a month ago or whenever it was, that the birth certificate posted on the White House website might be fraudulent, I started getting, as you might imagine, literally over 1,200 emails from people saying 'well that's proof, you should require the president to produce the original of his birth certificate in order to be on the ballot of Arizona.'
Arpaio's press conference more closely resembled an SNL parody than a serious investigation, and it was widely ridiculed for employing faulty "science" and drawing wild conclusions based on little more than technological anomalies.
Bennett is hardly the first person to propose removing Obama from the general election ballot this fall, but as secretary of state, he is in a position to actually act on those threats. Bennett's insistence that he is not a birther and is simply doing his due diligence as the state's top election official is a distinction without difference, as it ignores the fact that he is accepting as possibility that Obama's publicly available birth certificate is fraudulent.


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Universiti Putra Malaysia, Bahagian Komunikasi Korporat (2011) AMIC sets sights on Green Aviation.
The Aerospace Malaysian Innovation Centre (AMIC), a consortium-led project spearheaded by European Aeronautics Defence and Space Company (EADS), Rolls Royce, Composite Technology Research Malaysia (CTRM) and the Government of Malaysia convened its first board meeting on Monday, 14 Nov 2011, setting research priorities for upcoming projects. Science Advisor to Prime Minister Prof. Emeritus Datuk Dr Zakri Abdul Hamid and Chief Technical Officer of EADS Dr Jean Botti are the joint chairmen for the Board of directors. The centre is setting its sights on technology to develop jet fuel from algae, innovative new standards in aero structure manufacturing and sustainable green aeronautic materials as well as improved technologies for systems integration.
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|Universiti Putra Malaysia
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|30 Nov 2011 03:14
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You know, this whole shopping-for-a-holster migraine has me longing for the 5 month wait time for my CCL in the first place!
Ok, here's the rant. Any advice other than "calm down, Bunny" would be appreciated. :) Thanks.
So I get notified that for Sunday's BIT and Tuesday's Basic Pistol, I will need "a level 2 or 3 retention holster," among other things. WHY? Are we going to be hung upside-down and shaken to make sure our pistols don't move? But whatever. I went to the gun show Sunday morning and looked at every single booth (thanks for being so patient, ASSA9) and NOBODY HAD ONE for a Sig Sauer P239!
All I was using was a cheap plastic Fobus paddle holster for the range and OC, but that won't do now for a multitude of reasons.
So. I was thinking "well, just try and get a CC holster with level 2 retention" I need a CC holster anyway, why not kill 2 birds with 1 holster? You'd think it would be easy. Ok, I thought it would be easy. Boy was I in for a lesson.
Ok, I'm 5'4" on a good day. And while I'm not morbidly obese, there is NO ROOM in my waistband for IWB! I have a hip injury from ages ago, not to mention that it's a little inconvenient for me to do an ankle holster, especially if on the move or wearing my cowgirl boots. Shoulder rigs are hardly "conceal" worthy on me, especially with the cut of women's clothes today!
I tried buying men's jeans, men's shirts...my husband says...well never mind, but there are some disparaging remarks and referenced to Rosie O'Donnell and K.D. Lang. So that's not going so well.
I thought about a smartcarry, but my Sig doesn't have any external safeties AND I work with large dogs that jump on me a lot, and all I need is one claw to hook the wrong way and I'm afraid of blammo! Shooting off something that I would rather stay intact, like an artery or something.
So we're at OWB now, I guess. I plunked down $90 for aGalco Leather one today after the 4th salesguy at the gun shop finally seemed to know what he was talking about! (Is it just me, or are they getting dumber and less helpful?) So I have it on, and I don't like it. I still print, even with a button down shirt over my tank top. Even if I leave the button-down open. And I never wear button-downs, but honestly, how else to conceal now?
It's just frustrating. I went and bought 4 new pair of pants, all a size larger, just in the hopes that I find an IWB that's comfortable.
I'm considering a mumu at this point. Help! Maybe it's just hunger talking? I'm going to go eat dinner and check back in later.
Rant off.
PS: NO PURSE CARRY. Ever.


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IFF Opens New Manufacturing Facility In Singapore To Support Future Growth
International Flavors & Fragrances Inc. (NYSE: IFF), a leading global creator of flavors and fragrances for consumer products, today announced the opening of a new state-of-the-art liquid flavors and fragrances manufacturing plant in Jurong, Singapore. The higher-capacity, 12,000 square meter facility is part of a previously announced US$100 million investment in Greater Asia and replaces the Company's existing plant in the same area.
"Our continued investment in the Greater Asia region reflects our confidence in the future growth opportunities in this market both for our customers and for IFF," said Doug Tough, IFF Chairman and Chief Executive Officer. "We are committed to providing our customers with world-class support – the finest flavors and fragrances created under the most demanding quality standards to better serve our Asian customers. We are honored to further build on our over 40 year history in Singapore as an active supporter of its economy," he continued.
The new plant, with production capacity of up to 20,000 metric tons over time, was designed using industrial best practices in all aspects of its operation, allowing the Company to maximize productivity and efficiency while maintaining high product quality. In keeping with IFF's commitment to reduce its impact on the environment, the plant was built with automated processes that dramatically minimize usage of water, energy and cleaning chemicals. All waste water is treated on site to the highest industrial standards and the plant generates minimal solid waste. In addition to manufacturing liquid flavors and fragrances for the Greater Asia region generally, the plant will provide support to the Company's Center of Excellence for Functional Fragrances, which is housed in IFF's nearby Science Park creative facility.
Mr. Tan Choon Shian, Deputy Managing Director of the Singapore Economic Development Board, said "Singapore is delighted that a market-leader like IFF has chosen to establish its state-of-the-art green manufacturing facility and Centre of Excellence for functional fragrances here. This validates our pro-business environment and robust intellectual property protection for companies such as IFF to undertake proprietary manufacturing activities that will help them win in Asia. Singapore is also committed to developing a vibrant ecosystem of flavors and fragrances suppliers that can support the research and development activities of consumer goods companies to develop products that cater to the needs and preferences of Asian consumers."
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Discover your place of refuge
Ever wished you had a secret place you could run to, in order to escape the chaos of life? Or to simply catch your breath? Well, discover that such a place exists, and is waiting for you!Read More »
Ever wished you had a secret place you could run to, in order to escape the chaos of life? Or to simply catch your breath? Well, discover that such a place exists, and is waiting for you!Read More »
The more we discover who the Old Testament character of Jacob was, the more we may wonder why God would ever want to be associated with such a person, let alone have a relationship with him! We're getting to know "The God of Jacob."Read More »
Caught with no way out, many people have tried to bargain with God. "Lord, if you help me right now, I'll turn my life around!" But does God ever answer those types of prayers? Let's discuss Jacob's negotiation with God.Read More »
Each day we write another chapter in our own personal legacy. So when you finally leave this earth, what kind of story will you leave behind? Let's discuss how we want to be remembered, and that's as people who were loved!Read More »
What is the one thing you ask God for the most? Protection for your family? Food on the table? It's the conclusion of a study on "The Mercy Prayer."Read More »
A fresh water spring cannot quench our thirst if it accumulates in one spot. Instead it stagnates. And the same goes for God's mercy.Read More »
Jesus wants to shower you with His mercy. But first, He has some questions for you to answer. The two probing questions that Jesus asked of those looking for mercy reveal our faith and trust!Read More »
When the weight of life crushes down on us, and the pain is more than we can bear, our plea to God is "Why?" How our personal pain may be the perfect answer to the prayer; "Lord, have mercy."Read More »
There are events in life that call for justice. Other times, we're desperately seeking mercy. And almost every day, we're in need of grace!Read More »
If we ever doubt God's love, if we're ever uncertain about His grace, if we're ever unclear about His mercy, we need only look toward the cross! Jesus answered the most common prayer in the Bible, "Lord, have mercy."Read More »


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The Internet is abuzz thanks to the steamy, revealing blog, Scenes of a Sexual Nature. The posts leave nothing to the imagination, detailing all sorts of delicious – and sexual – secrets. The author behind the blog, NiceGirl, is a bit of an enigma, but manages to catch the eye of Mark Bell, an up-and-coming […]
Category Archive — Internet
Some Girls Do
By Meredith | Also posted in book reviews, clodagh murphy, contemporary, ireland, reading, romance
September 24, 2014 – 7:00 AM
Book News, Dec. 11th
By Meredith | Also posted in authors, book club, book news, classic literature, holidays, sarah maclean, TBR, YA
I don't know about you, bookworms, but I'm ready for snow. It's December and it's cold. Snow should be involved or else this weather is just no fun. Plus, how else will Santa get around in his sleigh if there's no snow? While I ponder that great question of our time, how about you ponder […]
December 11, 2010 – 10:00 AM
Flying Cars and Paperless Books
By Meredith | Also posted in blogs, books, children's literature, e-books, reading, reading habits, technology, writing, YA
Reading used to be fairly straightforward: you open the book and read the words on the page. But as technology advances and all sorts of gizmos and gadgets make their way into stores, the once-simple idea of reading is changing as well. A recent article in School Library Journal outlines the launch of a new […]
August 10, 2010 – 7:56 AM


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Start-up offers instant Windows bootup
New software will give you the option of starting Windows and wait--or booting Splashtop and be ready for action immediately.
Have you ever dreamed about turning on your Windows-based computer and having it instantly ready to work? A Silicon Valley start-up, Device VM, has developed software called Splashtop that, when prompted, will circumvent Windows and allow you to start watching a DVD in as little as five seconds. The Linux-based Splashtop is already available on Asus computers.
Read the full story on MIT Technology Review: "Instant bootup ".


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I saw Rascal slipping out the back door last night when I went to bed. I didn't hear him sneak back into the house during the middle of the night. This morning when I came into the living room, I didn't see Rascal. I woke up the kids and asked them if they knew where Rascal was.
Read the rest of the story and see photos of his hiding place at Uplifting Families.
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Is there a facility in Windows Server 2003 where i can check who is logged onto what workstation (Past or Present)?
I understand you can create logon scripts saying
echo %computer name%, %username% >> \\servername\filename\logon.log etc...
But that may cause problems when multiple users are trying to write to the log at the same time. Is there a progrmam or anything in Windows Server 2003 i can use?
Hope you can help


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ArQule Reports Fiscal 2012 Year End And Fourth Quarter Results
ArQule, Inc. (NASDAQ: ARQL) today announced its financial results for the year and for the fourth quarter ended December 31, 2012.
The Company reported a net loss of $10,872,000 or $0.18 per share, for the year ended December 31, 2012, compared with a net loss of $10,762,000, or $0.20 per share, for the year ended December 31, 2011. For the quarter ended December 31, 2012, the Company reported a net loss of $5,296,000 or $0.09 per share, compared with net income of $3,768,000, or $0.07 per share, for the quarter ended December 31, 2011.
At December 31, 2012, the Company had a total of approximately $130,599,000 in cash and marketable securities.
Operational MilestonesTivantinib (ARQ 197)
- Presentation of data at the 2012 Annual Meeting of the American Society of Clinical Oncology (ASCO) from a randomized, double-blind, controlled Phase 2 trial of tivantinib in second-line hepatocellular carcinoma (HCC) that met the primary endpoint of time to progression, with pronounced improvements observed in median overall survival and progression free survival in MET-high patients;
- Dosing of the first patient in the pivotal Phase 3 METIV-HCC trial of tivantinib as a single agent in second-line HCC MET-high patients in January 2013;
- Agreement with the U.S. Food and Drug Administration (FDA) on a Special Protocol Assessment (SPA) for the design of the METIV-HCC trial;
- Discontinuation of the Phase 3 MARQUEE trial of tivantinib and erlotinib in non-squamous non-small cell lung cancer (NSCLC), conducted by our partner Daiichi Sankyo Co., Ltd., following an interim analysis, with patients already on treatment and re-consented continuing to receive treatment;
- Permanent suspension of enrollment in the Phase 3 ATTENTION trial of tivantinib and erlotinib in non-squamous NSCLC in Asia conducted by our partner, Kyowa Hakko Kirin Co., Ltd., with patients already enrolled and re-consented continuing to receive treatment;
- Announcement of top-line data from the randomized Phase 2 signal generation trial of tivantinib in combination with irinotecan and cetuximab in second-line colorectal cancer (CRC) showing a trend of improvements in progression-free survival and objective response rate;
- Presentation of Phase 1b data at the ASCO Annual Meeting showing that the combination of tivantinib and sorafenib was well tolerated and that preliminary anti-tumor activity was observed in multiple patient extension cohorts, including HCC.
- Commencement of patient dosing in a Phase 1 clinical trial with ARQ 087, an orally bioavailable, multi-kinase inhibitor with pan-FGFR (fibroblast growth factor receptor) activity.
- timely progress in patient enrollment in the Phase 3 METIV-HCC trial;
- completion of patient enrollment in the Phase 2 KRAS-mutation positive NSCLC trial;
- completion and presentation of data analyses from the MARQUEE trial;
- data read-out from the ATTENTION trial by Kyowa Hakko Kirin expected in late 2013 or early 2014;
- presentation of final data from the randomized Phase 2 combination trial with irinotecan and cetuximab in colorectal cancer;
- support of ongoing clinical trials sponsored by the National Cancer Institute/Cancer Therapy Evaluation Program.
- enrollment of patients in the Phase 1 trial with ARQ 087;
- completion of patient enrollment in the Phase 1 trial with ARQ 092;
- screening of the Company's proprietary library of compounds as part of a drug discovery effort directed toward defined therapeutic targets.
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text: Take a photo tour of our House of Innovation Print Email Thomas J. Story PagesPrevious 6 of 23 Next View All Just off the kitchen Takeaway idea: Counters are for more than chopping and holding appliances. This granite-topped surface from DuPont contains a built-in trough for icing bottled drinks. Related Links Fabulous barn style by Monterey Bay Eco design goes glam in San Francisco A distinct interior in Menlo Park, Calif.


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Despite Muslim prohibitions, wine produced and sold from vineyards older than Roman times.
MEKNES, Morocco — Asked to brainstorm unlikely business plans, you might devise something more improbable than a winery in Muslim Morocco — perhaps a boat dealership for Bedouins? a sex shop in the Vatican? — but the list wouldn't be long.
More surprising still is the fact that Morocco's oldest winery, Celliers de Meknes, has made a brisk business of selling booze in a country where 98 percent of the population is forbidden to drink alcoholic beverages.
"We are tolerated," said Jean-Pierre Dehut, the export manager for Celliers de Meknes. "But the tolerance requires that we stay within certain boundaries."
Technically, those boundaries demarcate a zone so small it could squeeze the winery out of business. Moroccan law prohibits selling alcohol to Muslims — all but 2 percent of the country's 35 million people — and equally forbids Muslims from buying the stuff. Luckily for winemakers like Dehut , the rules are seldom enforced.
Taking a line that would make any legal pragmatist proud, Dehut concludes, "If it were illegal, we wouldn't exist anymore."
That's been a profitable supposition to make. The Celliers de Meknes sells some 30 million bottles of wine per year — 25 million of them right here in Morocco. The winery puts out bottles under esteemed appellations such as Guerrouane, Beni M'Tir and Les Coteaux de L'Atlas — the last trademark being Morocco's only Appellation d'Origine Controlee (AOC), a French system that ensures wines come from the precise geographical location advertised on their bottles.
But Dehut said the biggest domestic seller by far — 17 million bottles per year — is called Maghrebi, plastic-capped ultra-cheap stuff that has more in common with Colt 45 than it does Cabernet.
"It's an ordinary wine that's intended for Monsieur Tout le Monde," Dehut said, using a phrase that literally means "Mr. Everybody," but which may render better in English as "Joe Sixpack."
Morocco ranks far below the top three wine-producing countries Spain, France and Italy, which each grow more than 2 million tons of grapes per year, according to the California-based Wine Institute, a trade group that monitors the wine industry.
At just under a million tons annually, the United States stands in sixth place behind Turkey and China. Morocco, producing just 310,000 tons annually, ranks 30th worldwide.


text: Someone pointed this out to me and I figured I'd share it. It's a cover by Matchbox Twenty of 'The Smithereens - Girl Like You'. http://www.youtube.com/watch?v=97q0HY7oyCg I came accross it because I read that on Santana's new album Rob Thomas is doing a cover with him of 'Sunshine of Your Love'. He didn't strike me as that type of guy who could pull that off, but I thought he did a pretty good job with this one.


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Bruce McCulloch "Young Drunk Punk"
June 19, 2014
in TOsketchfest News Comments: 1
TOsketchfest presents YOUNG DRUNK PUNK, written and performed by Kids in the Hall funny-man Bruce McCulloch, and musical accompaniment by Brian Connelly of Shadowy Men on a Shadowy Planet, live onstage Tuesday, October 21, 2014. This special live performance will launch McCulloch's new book Let's Start a Riot: How A Young Drunk Punk became A Hollywood Dad, and includes a book signing and post-show reception.
Tuesday, October 21, 2014
8pm – Isabel Bader Theatre (93 Charles St W)
Tickets: $39 (Show only) / $55 (including a copy of "Let's Start a Riot: How A Young Drunk Punk became A Hollywood Dad")
All tix assigned seating
Pricing does not include HST and fees
Advance tickets available ONLINE ONLY
Adult Content
Running Time: Approx. 70 minutes, No Intermission
Isabel Bader Theatre is an accessible venue
1 Comment(add yours)
Sounds good to me. Just saw Bruce and the gang at Royal Oak, Michigan show. Made me feel young again. Or younger.


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My hermit has molted, and I spray him every day to give him moisture. I also put a wet towel in his cage. When I saw the mold this morning, I removed the towel and didn't spray him. How can I get rid of the mold?
My hermit has molted, and I spray him every day to give him moisture. I also put a wet towel in his cage. When I saw the mold this morning, I removed the towel and didn't spray him. How can I get rid of the mold?
You can give it a try,the fuzzy mold is a sign that it is in advanced stages, so it is important to isolate him from the others, then do the following,
To treat mould and fungus spots or infection, gently bathe the hermit crab in approximately one half (1/2) of a teaspoon of aquarium salt(Instant Ocean or Doc Fishwell are the best to a quart/Litre of dechlorinated water., as well as in the saline solution treatment, to put a drop of StressCoat in it, the aloe vera is helpful in aiding recovery.
But mold on hermit crabs is usually fatal as it gets in the layers of the exoskeleton.
Do a complete bedding/substrate change, wash all bowls and quarantine container in a aquarium salt/vinigar solution diluted with dechlorinated water.lower your humidity slightly and do not mist make sure you in this case take the shed exoskeleton and put in fresh cuttle bone to replace the calcium he would have gotten from the molted shell, but you want to get rid of everything and start fresh.
The odds are not good as your crab is vunerable at this time as its soft moist shell can be open to shell disease, black spot, etc at this time, you can give it a try but it may not make it because the mold is usually fatal even to crabs that are not molting
mold is a sign that the tank has too much moisture. take out the crab, change the bedding, clean the tank with a mild bleach solution and make sure to rinse well, put new bedding and the crab back in. mold isn't going to hurt the crab but it looks gross and could start to smell. maybe instead of spraying him and adding a wet towel you could just get a soaking bowl, one with fresh dechlorinated water and the other with dechlorinated salt water. Thats what i do. and once a week i give my crabs a bath, i put them in a large bucket of dechlorinated salt water (i put in a rock so they can climb out of the water too if they wish) and i have never had a humidity problem or a crab health issue in my tank!
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Reviewed Red Beans and Rice
Jun 23, 2012 in Food Network Community Toolbox on FoodNetwork.com
"Good recipe. 10 cups of stock is way too much. 8 cups was still rather soupy. I followed the recipe except I used Andouille sausage and I did add more onion and green pepper and celery than called for and also used more garlic. Used a smoked pork hock instead of a ham hock. Very tasty!""