The PhLigel and BuLigel blocks also performed very well in other nucleophilic addition reactions. For these reactions, the organolithium gels were prepared and then stored for 10-30 s before use in the reactions shown -good conversions to products 3, 5 and 7-9 (75-79%) were obtained from reactions with 2′-methoxyacetophenone 1, benzophenone 4 and N-benzylideneaniline 6 (Fig. ). It was important to show that the C36H74 gelator can be readily separated from the products. In general, most of the C36H74 gelator can be removed in the work-up by precipitation and filtration. Standard flash column chromatography can then be used to remove the final traces of the C36H74 gelator, eluting first with hexane to remove C36H74 and then with 1:1 hexane-dichloromethane to elute the product. Using this method, a 98% isolated yield of alcohol 5 was obtained from a PhLigel block and benzophenone 4 (Fig. ). The same approach was used by Buchwald and co-workers to remove the residual paraffin from reactions using their paraffin capsules. The PhLigel and BuLigel blocks were then used in a wider array of synthetic applications, including more challenging reactions (Fig. ). For example, reaction of each of the PhLigel and BuLigel blocks with benzonitrile 10 followed by hydrolysis resulted in the formation of ketones 4 and 11 in 96% and 87% NMR yields respectively (Fig. ). The preparation of a PhLigel block was scaled up (to 9.5 mmol of PhLi encapsulated, see ESI) and this PhLigel block was used in the synthesis of 0.87 g of the anticholinergic and antihistamine drug Orphenadrine 14. Reaction of the PhLigel with 2-methylbenzaldehyde 12 was performed under ambient conditions in air to give alcohol 13 in 95% isolated yield and, after Nalkylation with 2-(N,N-dimethylamino)ethylchloride, Orphenadrine 14 was obtained in 68% yield over the two steps (Fig. ). To show that the organolithium gel blocks are also compatible with other types of reactions, a bromine-lithium exchange reaction was performed with 4-bromoanisole 15 using a BuLigel block at -78 °C under an inert atmosphere followed by trapping the intermediate aryllithium with 4-methoxybenzaldehyde 16 to give alcohol 17 in 99% isolated yield (Fig. ). The BuLigel block was also successfully used to generate an ylid from phosphonium bromide 18 and deployed in a Wittig reaction with benzophenone 4 to give alkene 19 in 98% isolated yield (Fig. ). The widely used strong base LDA 21 was readily prepared from diisopropylamine 20 and used in an enolate α-alkylation ). Finally, we successfully utilized both the PhLigel and BuLigel blocks in a three-step, double α-C-H functionalization of pyrrolidine under inert conditions (Fig. ). In the first step, using Seidel's approach with the PhLigel block, deprotonation of the NH proton in pyrrolidine 25 by PhLi followed by hydride transfer to benzophenone 4 as a hydride acceptor and addition of PhLi to the in situ-generated imine provided 2-phenylpyrrolidine 26 in 37% isolated yield. 2-Phenylpyrrolidine 26 was Boc-protected and then, following a method reported by O'Brien and Coldham, 48 benzylic lithiation using a BuLigel block at 0 °C and subsequent reaction with ethyl chloroformate gave α,α-disubstituted pyrrolidine 28 in 78% isolated yield.