Carroll Kyler J, Burger Thomas, Langenegger Lukas, Chavez Steven, Hunt Sean T, Román-Leshkov Yuriy, Brushett Fikile R
Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave, Cambridge, MA, 02139, USA.
Department of Chemistry, Technical University of Munich, Lichtenbergstraße 4, 85748, Garching, Germany.
ChemSusChem. 2016 Aug 9;9(15):1904-10. doi: 10.1002/cssc.201600290. Epub 2016 Jun 23.
Electrocatalytic hydrogenation (ECH) is a sustainable pathway for the synthesis of value-added organic compounds, provided affordable catalysts with high activity, selectivity and durability are developed. Here, we synthesize Cu/C, Ni/C, and CuNi/C nanoparticles and compare their performance to Pt/C, Ru/C, PtRu/C for the ECH of hydroxyacetone, a bio-derived feedstock surrogate containing a carbonyl and a hydroxyl functional group. The non-precious metal electrocatalysts show promising conversion-time behavior, product selectivities, and Faradaic efficiencies. Ni/C forms propylene glycol with a selectivity of 89 % (at 80 % conversion), while Cu/C catalyzes ECH (52 % selectivity) and hydrodeoxygenation (HDO, 48 % selectivity, accounting for evaporation). CuNi/C shows increased turnover frequencies but reduced ECH selectivity (80 % at 80 % conversion) as compared to the Ni/C catalyst. Importantly, stability studies show that the non-precious metal catalysts do not leach at operating conditions.
电催化氢化（ECH）是合成高附加值有机化合物的一条可持续途径，前提是要开发出具有高活性、选择性和耐久性且价格合理的催化剂。在此，我们合成了铜/碳（Cu/C）、镍/碳（Ni/C）和铜镍/碳（CuNi/C）纳米颗粒，并将它们在对羟基丙酮（一种含有羰基和羟基官能团的生物衍生原料替代物）进行电催化氢化反应中的性能与铂/碳（Pt/C）、钌/碳（Ru/C）、铂钌/碳（PtRu/C）进行了比较。这些非贵金属电催化剂表现出了令人期待的转化率-时间行为、产物选择性和法拉第效率。镍/碳形成丙二醇的选择性为89%（转化率为80%时），而铜/碳催化电催化氢化反应（选择性为52%）和加氢脱氧反应（HDO，选择性为48%，包括蒸发所致）。与镍/碳催化剂相比，铜镍/碳的周转频率有所提高，但电催化氢化反应的选择性降低（转化率为80%时为80%）。重要的是，稳定性研究表明，这些非贵金属催化剂在操作条件下不会浸出。
