期刊
ACS APPLIED NANO MATERIALS
卷 5, 期 8, 页码 10174-10182出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.2c00323
关键词
Cu-CuS; BM; electrocatalysis; glycerol; formate; selectivity
资金
- National Natural Science Foundation of China [2177060378, 21521005]
- Program for Changjiang Scholars and Innovative Research Teams in Universities [IRT1205]
- Fundamental Research Funds for the Central Universities [12060093063, XK1803-05]
This study provides a simple method for the development of a high-activity non-noble metal catalyst for the oxidation of glycerol to formate. CuS nanosheet arrays are grown on a brass mesh, and copper nanoparticles are uniformly dotted on the CuS nanosheets to form Cu-CuS/BM. Cu-CuS/BM exhibits excellent activity and stability, with high selectivity and Faradaic efficiency for formate production.
This work provides a simple method for the development of a high-activity non-noble metal catalyst for the oxidation of glycerol (GLY) to formate. CuS nanosheet arrays are grown in situ on the brass mesh by low-temperature sulfuration, and then copper nanoparticles are uniformly dotted on CuS nanosheets through disproportionation reaction. As-fabricated Cu-CuS/BM is used for glycerol oxidation reaction (GOR), and the current density can reach 10 mA.cm(-2) when the potential is 1.37 V vs RHE. A high selectivity of 86.0% and a Faradaic efficiency of 90.4% for formate production are achieved, and the average selectivity of 20 consecutive cycles of electrolysis is 82.6%, confirming the excellent activity and stability of Cu-CuS/BM. The formation of formate as the main oxidation product that conforms to the primary alcohol oxidation path is proved through high-performance liquid chromatography and in situ Fourier transform infrared spectroscopy. The mechanism of GOR induced by Cu-CuS/BM is proposed through density functional theory calculation and X-ray photoelectron spectroscopy analysis, in which the combination of copper nanoparticles and CuS significantly enhances the adsorption for GLY, and Cu(II) produced during the GOR facilitates the adsorption for OH- to form Cu(II)-OHads on the catalyst surface, which is beneficial to the oxidation of absorbed GLY.
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