4.6 Article

Design the PdCu/TaN-C electrocatalyst with core-shell structure having high efficiency for methanol and formic acid oxidation reactions

期刊

ELECTROCHIMICA ACTA
卷 383, 期 -, 页码 -

出版社

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2021.138365

关键词

PdCu/TaN-C; Methanol oxidation reactions; Formic acid oxidation reactions; Core-shell structure; Bi-functional catalysts

资金

  1. National Natural Science Foundation of China [22075225, 21706203, 22038011]
  2. Special Guidance Funds for the Construction of World-Class Universities (Disciplines) and Characteristic Development in Central Universities [PY3A076]
  3. China Postdoctoral Science Foundation [2020T130508, 2019M660258, 2019M663731]
  4. Natural Science Basic Research Plan in Shaanxi Province of China [2017JQ2030, 2020JQ023]
  5. Fundamental Research Funds for the Central Universities (Xi'an Jiaotong University) [cxtd2017004, xjj2018035]
  6. Shaanxi Creative Talents Promotion Plan-Technological Innovation Team [2019TD-039]
  7. Joint Laboratory of Xi'an Jiaotong Univ
  8. Shaanxi Coal Chemical Industry Technology Research Institute Co. Ltd

向作者/读者索取更多资源

The PdCu/TaN-C catalyst showed high catalytic performance for MOR and FAOR, with significantly enhanced reaction kinetics, anti-CO poisoning ability, and stability. DFT calculations revealed weakened CO adsorption intensity and enhanced OH binding intensity on its surface, contributing to the removal of adsorbed CO and enhancement of anti-CO poisoning ability.
For the first time, PdCu/TaN-C catalyst with a special core-shell structure is assembled, which exhibits high catalytic performance for methanol oxidation reaction (MOR) in alkaline medium (1326.95 A g(Pd)(-1)) and formic acid oxidation reaction (FAOR) in acidic medium (1052.63 A g(Pd)(-1)), 6.3 and 4.9 times those of the commercial Pd/C, respectively. According to the results of Tafel, Electrochemical Impedance Spectroscopy (EIS), CO stripping and chronoamperometry (CA), it is revealed that the reaction kinetics, anti-CO poisoning ability and stability of PdCu/TaN-C for MOR and FAOR are all enhanced significantly. Density Functional Theory (DFT) calculations also indicate that the adsorption intensity of CO is weakened and the binding intensity of OH is enhanced on the Pd3Cu1/TaN(001) surface, which are beneficial to the removal of adsorbed CO and enhancement of the anti-CO poisoning ability. Combined with the characterization analysis and theoretical calculations, the good catalytic performance of PdCu/TaN-C for MOR and FAOR can be attributed to the unique electronic structure and morphology from the effective interface, geometric effects and proper d-band center. (C) 2021 Elsevier Ltd. All rights reserved.

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