Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy
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 vacan...
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| Published in | Nature communications Vol. 11; no. 1; pp. 1664 - 9 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
03.04.2020
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | 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 CoSe
2
nanobelts for /coxygen evolution catalysis, and the resulted CoSe
2
-D
Fe
–V
Co
exhibits much higher catalytic activity than other defect-activated CoSe
2
and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co
2
site that is adjacent to the V
Co
-nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co
2
to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔE
OH
) without changing ΔE
O
, 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.
While electronic-structure engineering lies at the heart of catalyst design, most previous studies utilize only one technique to tune the electronic states. Here, authors demonstrate that Fe doping and Co vacancy work synergistically to approach the activity limit of CoSe
2
for oxygen evolution reaction. |
|---|---|
| AbstractList | 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.While electronic-structure engineering lies at the heart of catalyst design, most previous studies utilize only one technique to tune the electronic states. Here, authors demonstrate that Fe doping and Co vacancy work synergistically to approach the activity limit of CoSe2 for oxygen evolution reaction. While electronic-structure engineering lies at the heart of catalyst design, most previous studies utilize only one technique to tune the electronic states. Here, authors demonstrate that Fe doping and Co vacancy work synergistically to approach the activity limit of CoSe2 for oxygen evolution reaction. 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 CoSe 2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe 2 -D Fe –V Co exhibits much higher catalytic activity than other defect-activated CoSe 2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co 2 site that is adjacent to the V Co -nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co 2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔE OH ) without changing ΔE O , 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. 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.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. 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 CoSe 2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe 2 -D Fe –V Co exhibits much higher catalytic activity than other defect-activated CoSe 2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co 2 site that is adjacent to the V Co -nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co 2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔE OH ) without changing ΔE O , 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. While electronic-structure engineering lies at the heart of catalyst design, most previous studies utilize only one technique to tune the electronic states. Here, authors demonstrate that Fe doping and Co vacancy work synergistically to approach the activity limit of CoSe 2 for oxygen evolution reaction. |
| ArticleNumber | 1664 |
| Author | Zhao, Huijun Ma, Jianmin Dou, Yuhai Yin, Huajie He, Chun-Ting Zhang, Lei Al-Mamun, Mohammad |
| Author_xml | – sequence: 1 givenname: Yuhai orcidid: 0000-0003-2549-1400 surname: Dou fullname: Dou, Yuhai organization: Centre for Clean Environment and Energy, Gold Coast Campus, Griffith University – sequence: 2 givenname: Chun-Ting surname: He fullname: He, Chun-Ting organization: Key Laboratory of Functional Small Organic Molecule, Ministry of Education, College of Chemistry and Chemical Engineering, Jiangxi Normal University – sequence: 3 givenname: Lei surname: Zhang fullname: Zhang, Lei organization: Centre for Clean Environment and Energy, Gold Coast Campus, Griffith University – sequence: 4 givenname: Huajie orcidid: 0000-0002-9036-9084 surname: Yin fullname: Yin, Huajie organization: Centre for Clean Environment and Energy, Gold Coast Campus, Griffith University – sequence: 5 givenname: Mohammad orcidid: 0000-0001-8201-4278 surname: Al-Mamun fullname: Al-Mamun, Mohammad organization: Centre for Clean Environment and Energy, Gold Coast Campus, Griffith University – sequence: 6 givenname: Jianmin surname: Ma fullname: Ma, Jianmin organization: School of Physics and Electronics, Hunan University – sequence: 7 givenname: Huijun orcidid: 0000-0002-3028-0459 surname: Zhao fullname: Zhao, Huijun email: h.zhao@griffith.edu.au organization: Centre for Clean Environment and Energy, Gold Coast Campus, Griffith University, Centre for Environmental and Energy Nanomaterials, CAS Centre for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences |
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| ContentType | Journal Article |
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| DOI | 10.1038/s41467-020-15498-0 |
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| Title | Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy |
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