Electrocatalytic Hydrogenation of Oxygenates using Earth-Abundant Transition-Metal Nanoparticles under Mild Conditions

被引:58
作者
Carroll, Kyler J. [1 ]
Burger, Thomas [1 ,2 ]
Langenegger, Lukas [1 ,3 ]
Chavez, Steven [1 ]
Hunt, Sean T. [1 ]
Roman-Leshkov, Yuriy [1 ]
Brushett, Fikile R. [1 ]
机构
[1] MIT, Dept Chem Engn, 77 Massachusetts Ave, Cambridge, MA 02139 USA
[2] Tech Univ Munich, Dept Chem, Lichtenbergstr 4, D-85748 Garching, Germany
[3] ETH, Inst Chem & Bioengn, Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland
基金
美国国家科学基金会;
关键词
electrocatalysis; heterogeneous catalysis; hydrogenation; nickel; renewable resources; LIQUID FUELS; CATALYSTS; HYDRODEOXYGENATION; BIOMASS; HYDROGENOLYSIS; DIMETHYLFURAN; ELECTRODES; EVOLUTION; CARBON;
D O I
10.1002/cssc.201600290
中图分类号
O6 [化学];
学科分类号
070301 [无机化学];
摘要
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.
引用
收藏
页码:1904 / 1910
页数:7
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