Selective conversion of biomass derivatives to value-added chemicals is an ongoing catalytic challenge. Often, high pressures of hydrogen (H2) and/or high temperatures are required to make the process viable. In this work, we developed a C-AuPd catalyst that is relatively easy to synthesize for the selective conversion of ethyl levulinate (EL) and aliphatic amines to analogous pyrrolidones, important pharmaceutical intermediates and surfactants, under ambient pressure H2. To make the process more sustainable, we demonstrated that C-AuPd is also extremely active for ammonia borane (AB) methanolysis, with one of the highest ever reported TOF values for a Pd-based catalyst of 122 mol mol-1AuPd min-1. The H2 produced from AB methanolysis was demonstrated to directly be used in the conversion of EL with no loss in activity, over the same C-AuPd catalyst. The most active catalyst found in both reactions, C-Au66Pd34, can be reused at least ten times for AB methanolysis and five times for ethyl levulinate reductive amination, with minimal loss in activity in both cases. Therefore, this catalyst, both easy to synthesize and extremely reusable, establishes a more sustainable process under mild operating conditions, while adding to the feasibility of using ambient pressure H2 in chemical conversions. This work, builds upon work in our group on other MPd catalysts, like AgPd, and the role of catalyst design in both systems will be discussed for improving catalyst activity, stability, and sustainablitiy.

Toward more sustainable MPd (M = Au, Ag) catalysis for dehydrogenation/hydrogenation reactions through nanomaterials design

2019 Spring National Meeting

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