Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 32, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202206588
Keywords
Adsorption; Electrocatalysis; Nickel; Orbital Interactions; Valence Electrons
Categories
Funding
- National Natural Science Foundation of China [22002046, 91963109]
- Fundamental Research Funds for the Central Universities [2020kfyXJJS063]
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In this study, the valence-electron arrangement of Ni active centers was controlled by using Ni-vacancy-enriched Ni3N. The Ni vacancies promoted the valence-electron delocalization of OH-adsorption centers and weakened the binding of H-adsorption centers, leading to a 15-fold enhancement in mass activity compared to Ni3N without vacancies. This research demonstrates the potential of finely tuning the valence-electron arrangement for designing efficient catalysts.
The valence-electron arrangement of heterogeneous catalysts can significantly affect the binding behavior of absorbates. However, it remains a challenge to understand the role of the valence-electron arrangement in electrocatalysis, which limits its utilization as a tool to design efficient electrocatalysts. Here, we describe experiments in which the valence-electron arrangement of Ni active centers for hydrogen oxidation is controlled precisely by using Ni-vacancy-enriched Ni3N as a platform. These Ni vacancies can promote the valence-electron delocalization of OH-adsorption centers to enhance the Ni ds-O 2p valence-electron-orbital interaction with elevated OH adsorption. Meanwhile, the deficit of valence-electrons of H-adsorption centers at Ni vacancies can lower Ni ds-H 1s interaction with weakened H binding. Relative to Ni3N poor in vacancies, the Ni-vacancy-enriched Ni3N showed a mass activity enhanced by 15-fold. This strategy paves a rational way to design efficient catalysts by finely tuning the valence-electron arrangement.
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