Open AccessPorous PdWM (M = Nb, Mo and Ta) Trimetallene for High C1 Selectivity in Alkaline Ethanol Oxidation Reaction
Author(s) -
Qin Yingnan,
Huang Hao,
Yu Wenhao,
Zhang Haonan,
Li Zhenjiang,
Wang Zuochao,
Lai Jianping,
Wang Lei,
Feng Shouhua
Publication year - 2022
Publication title -
advanced science
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.388
H-Index - 100
ISSN - 2198-3844
DOI - 10.1002/advs.202103722
Subject(s) - selectivity , fourier transform infrared spectroscopy , chemistry , adsorption , kinetics , ethanol , bond cleavage , valence (chemistry) , nuclear chemistry , inorganic chemistry , catalysis , chemical engineering , organic chemistry , physics , quantum mechanics , engineering
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 mg Pd −1 ) and C1 selectivity (55.5%) of Pd 50 W 27 Nb 23 /C trimetallene, obtained after optimizing the compositions and proportions of porous PdWM, outperform those of commercial Pt/C (1.3 A mg Pt −1 , 5.9%), Pd/C (5.0 A mg Pd −1 , 7.2%), and Pd 97 W 3 /C bimetallene (9.5 A mg Pd −1 , 14.1%). The mechanism by which Pd 50 W 27 Nb 23 /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 CH 3 CH 2 OH and oxophilic high‐valence Nb accelerates the subsequent oxidation of CO and CH x species. Moreover, Nb promotes the cleavage of CC bonds and increases the C1 selectivity. Pd 60 W 28 Mo 12 /C and Pd 64 W 27 Ta 9 /C trimetallene synthesized by the same method also exhibit excellent EOR performance.