Advanced Science (Feb 2022)

Porous PdWM (M = Nb, Mo and Ta) Trimetallene for High C1 Selectivity in Alkaline Ethanol Oxidation Reaction

  • Yingnan Qin,
  • Hao Huang,
  • Wenhao Yu,
  • Haonan Zhang,
  • Zhenjiang Li,
  • Zuochao Wang,
  • Jianping Lai,
  • Lei Wang,
  • Shouhua Feng

DOI
https://doi.org/10.1002/advs.202103722
Journal volume & issue
Vol. 9, no. 5
pp. n/a – n/a

Abstract

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Abstract Direct ethanol fuel cells are among the most efficient and environmentally friendly energy‐conversion devices and have been widely focused. The ethanol oxidation reaction (EOR) is a multielectron process with slow kinetics. The large amount of by‐product generated by incomplete oxidation greatly reduces the efficiency of energy conversion through the EOR. In this study, a novel type of trimetallene called porous PdWM (M = Nb, Mo and Ta) is synthesized by a facile method. The mass activity (15.6 A mgPd−1) and C1 selectivity (55.5%) of Pd50W27Nb23/C trimetallene, obtained after optimizing the compositions and proportions of porous PdWM, outperform those of commercial Pt/C (1.3 A mgPt−1, 5.9%), Pd/C (5.0 A mgPd−1, 7.2%), and Pd97W3/C bimetallene (9.5 A mgPd−1, 14.1%). The mechanism by which Pd50W27Nb23/C enhances the EOR performance is evaluated by in situ Fourier transform infrared spectroscopy and density functional theory calculations. It is found that W and Nb enhance the adsorption of CH3CH2OH and oxophilic high‐valence Nb accelerates the subsequent oxidation of CO and CHx species. Moreover, Nb promotes the cleavage of CC bonds and increases the C1 selectivity. Pd60W28Mo12/C and Pd64W27Ta9/C trimetallene synthesized by the same method also exhibit excellent EOR performance.

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