Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

View/ Open
File version
Version of Record (VoR)
Author(s)
Dou, Y
He, CT
Zhang, L
Yin, H
Al-Mamun, M
Ma, J
Zhao, H
Year published
2020
Metadata
Show full item recordAbstract
Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe2-DFe–VCo exhibits much higher catalytic activity than other defect-activated CoSe2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co2 site that is adjacent ...
View more >Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe2-DFe–VCo exhibits much higher catalytic activity than other defect-activated CoSe2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co2 site that is adjacent to the VCo-nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔEOH) without changing ΔEO, and consequently lowering the catalytic overpotential. The proper combination of multiple defect structures is promising to unlock the catalytic power of different catalysts for various electrochemical reactions.
View less >
View more >Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe2-DFe–VCo exhibits much higher catalytic activity than other defect-activated CoSe2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co2 site that is adjacent to the VCo-nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔEOH) without changing ΔEO, and consequently lowering the catalytic overpotential. The proper combination of multiple defect structures is promising to unlock the catalytic power of different catalysts for various electrochemical reactions.
View less >
Journal Title
Nature Communications
Volume
11
Issue
1
Copyright Statement
© The Author(s) 2020. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
Subject
Chemical sciences