At the outset of our studies, various reaction conditions were tested for the electrochemical reduction of p-hydroxy benzylidene acetone 1a (Table ). As hydrogen gas production is a side reaction for this system, FE was used to determine the fraction of electrons involved in the target ECH, and at the same time as to assess the extent of the HER side reaction. The commercially supplied Ni foam was first activated by sonication in H2SO4 (3 M aq.) for 10 min. This activation was carried out a single time on the commercially supplied foam, after purchasing. When the electrochemical reduction reaction of 1a was carried out under the same conditions as in our previous study on the reduction of alkynes (vide supra, Scheme 1b), namely a mixture 1:1 (v/v) of acetone and H2SO4 (0.5 M aq.), only a moderate yield of the product was obtained, and also a very low FE was observed (Table , entry 1). This was not surprising, as these conditions were optimized for the selective semihydrogenation of alkynes to alkenes, and any further hydrogenation to form saturated derivatives occurred at much lower rates. A significant improvement in the yield was observed when MeOH was used as the organic cosolvent instead of acetone, although the FE of this reaction was low (Table , entry 2). By increasing the MeOH/H2SO4 ratio to 3:1 (v/v), the FE were improved; this also allowed us to decrease the applied potential to -0.9 V (Table , entries 3 and 4). Under these conditions a good yield of 78% was obtained, with a FE of 4%. The concentration of H2SO4 was lowered to 0.19 M, which provided a good yield of 77% (Table , entry 5).