Journal
ADVANCED MATERIALS
Volume 34, Issue 16, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202106541
Keywords
cation vacancy engineering; electrocatalysis; green production; hydrogen peroxide production; oxygen reduction reaction
Categories
Funding
- Australian Research Council Discovery Early Career Researcher Award [DE220100676]
- FH Loxton Fellowship of the USYD
- National Natural Science Foundation of China [12005227]
- University of Science and Technology of China - Ministry of Science and Technology of China [2017YFA0204904]
- Australian Research Council [DE220100676] Funding Source: Australian Research Council
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Electrocatalytic hydrogen peroxide synthesis via two-electron oxygen reduction reaction pathway is becoming increasingly important due to its green production process. Introducing cationic vacancies on nickel phosphide as a proof-of-concept to regulate the catalyst's properties has led to efficient H2O2 electrosynthesis. The created Ni cationic vacancies enriched Ni2-xP-V-Ni electrocatalyst exhibits remarkable 2e ORR performance and long-term durability, with optimized geometric and electronic structures. Cation vacancy engineering is believed to be an effective strategy for creating active heterogeneous catalysts with atomic precision.
Electrocatalytic hydrogen peroxide (H2O2) synthesis via the two-electron oxygen reduction reaction (2e ORR) pathway is becoming increasingly important due to the green production process. Here, cationic vacancies on nickel phosphide, as a proof-of-concept to regulate the catalyst's physicochemical properties, are introduced for efficient H2O2 electrosynthesis. The as-fabricated Ni cationic vacancies (V-Ni)-enriched Ni2-xP-V-Ni electrocatalyst exhibits remarkable 2e ORR performance with H2O2 molar fraction of >95% and Faradaic efficiencies of >90% in all pH conditions under a wide range of applied potentials. Impressively, the as-created V-Ni possesses superb long-term durability for over 50 h, suppassing all the recently reported catalysts for H2O2 electrosynthesis. Operando X-ray absorption near-edge spectroscopy (XANES) and synchrotron Fourier transform infrared (SR-FTIR) combining theoretical calculations reveal that the excellent catalytic performance originates from the V-Ni-induced geometric and electronic structural optimization, thus promoting oxygen adsorption to the 2e ORR favored end-on configuration. It is believed that the demonstrated cation vacancy engineering is an effective strategy toward creating active heterogeneous catalysts with atomic precision.
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