硼氮共掺杂纳米金刚石上二氧化碳选择性电化学还原为乙醇。
Selective Electrochemical Reduction of Carbon Dioxide to Ethanol on a Boron- and Nitrogen-Co-doped Nanodiamond.
机构信息
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), Faculty of Chemical, Environmental and Biological Science and Technology, Dalian University of Technology, Dalian, 116024, China.
School of Physics and Opto-Electronic Technology, Dalian University of Technology, Dalian, 116024, China.
出版信息
Angew Chem Int Ed Engl. 2017 Dec 4;56(49):15607-15611. doi: 10.1002/anie.201706311. Epub 2017 Oct 24.
Electrochemical reduction of CO to ethanol, a clean and renewable liquid fuel with high heating value, is an attractive strategy for global warming mitigation and resource utilization. However, converting CO to ethanol remains great challenge due to the low activity, poor product selectivity and stability of electrocatalysts. Here, the B- and N-co-doped nanodiamond (BND) was reported as an efficient and stable electrode for selective reduction of CO to ethanol. Good ethanol selectivity was achieved on the BND with high Faradaic efficiency of 93.2 % (-1.0 V vs. RHE), which overcame the limitation of low selectivity for multicarbon or high heating value fuels. Its superior performance was mainly originated from the synergistic effect of B and N co-doping, high N content and overpotential for hydrogen evolution. The possible pathway for CO reduction revealed by DFT computation was CO →*COOH→*CO→*COCO→*COCH OH→*CH OCH OH→CH CH OH.
电化学还原 CO 为乙醇，这是一种清洁可再生的高发热值液体燃料，对于缓解全球变暖及资源利用具有吸引力。然而，由于电催化剂活性低、产物选择性和稳定性差，将 CO 转化为乙醇仍然是一个巨大的挑战。在此，报道了硼和氮共掺杂纳米金刚石（BND）作为高效稳定的电极，用于选择性还原 CO 为乙醇。BND 上实现了良好的乙醇选择性，法拉第效率高达 93.2%（相对于 RHE，-1.0 V），克服了多碳或高热值燃料选择性低的局限性。其优异的性能主要源于 B 和 N 共掺杂、高 N 含量和析氢过电势的协同作用。通过 DFT 计算揭示的 CO 还原的可能途径为 CO →*COOH→*CO→*COCO→*COCH OH→*CH OCH OH→CH CH OH。
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