期刊
ACS CATALYSIS
卷 10, 期 12, 页码 6741-6752出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c01498
关键词
biomass conversion; glycerol oxidation; spinel oxides; formic acid; electrocatalysis; fuel cell
资金
- National Science Foundation (NSF) [DMR-1508558]
- China Scholarship Council (CSC)
- National Natural Science Foundation of China (NSFC) [51872035]
- Fundamental Research Funds for the Central Universities [DUT19LAB20]
- Xingliao Support Program for Young Talent of Liaoning Province [XLYC1807002]
- Xinghai Scholarship of Dalian University of Technology
- National Key Research Development Program of China [2016YFB0101201]
- Great Lakes Bioenergy Research Center, U.S. Department of Energy [DE-SC0018409]
- NSF through the University of Wisconsin Materials Research Science and Engineering Center [DMR1720415]
The electrochemical oxidation of abundantly available glycerol for the production of value-added chemicals, such as formic acid, could be a promising approach to utilize glycerol more effectively and to meet the future demand for formic acid as a fuel for direct or indirect formic acid fuel cells. Here we report a comparative study of a series of earth-abundant cobalt-based spinel oxide (MCo2O4 , M = Mn, Fe, Co, Ni, Cu, and Zn) nanostructures as robust electrocatalysts for the glycerol oxidation to selectively produce formic acid. Their intrinsic catalytic activities in alkaline solution follow the sequence of CuCo2O4 > NiCo2O4 > CoCo2O4 > FeCo2O4 > ZnCo2O4 > MnCo2O4 . Using the best-performing CuCo2O4 catalyst directly integrated onto carbon fiber paper electrodes for the bulk electrolysis reaction of glycerol oxidation (pH = 13) at the constant potential of 1.30 V vs reversible hydrogen electrode (RHE), a high selectivity of 80.6% for formic acid production and an overall Faradaic efficiency of 89.1% toward all value-added products were achieved with a high glycerol conversion of 79.7%. Various structural characterization techniques confirm the stability of the CuCo2O4 catalyst after electrochemical testing. These results open up opportunities for studying earth-abundant electrocatalysts for efficient and selective oxidation of glycerol to produce formic acid or other value-added chemicals.
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