Engineering Single-Atom Electrocatalysts for Enhancing Kinetics of Acidic Volmer Reaction
The design of active and low-cost electrocatalyst for hydrogen evolution reaction (HER) is the key to achieving a clean hydrogen energy infrastructure. The most successful design principle of hydrogen electrocatalyst is the activity volcano plot, which is based on Sabatier principle and has been used to understand the exceptional activity of noble metal and design of metal alloy catalysts. However, this application of volcano plot in designing single-atom electrocatalysts (SAEs) on nitrogen doped graphene (TM/N4C catalysts) for HER has been less successful due to the nonmetallic nature of the single metal atom site. Herein, by performing ab initio molecular dynamics simulations and free energy calculations on a series of SAEs systems (TM/N4C with TM = 3d, 4d, or 5d metals), we find that the strong charge-dipole interaction between the negatively charged *H intermediate and the interfacial H2O molecules could alter the transition path of the acidic Volmer reaction and dramatically raise its kinetic barrier, despite its favorable adsorption free energy. Such kinetic hindrance is also experimentally confirmed by electrochemical measurements. By combining the hydrogen adsorption free energy and the physics of competing interfacial interactions, we propose a unifying design principle for engineering the SAEs used for hydrogen energy conversion, which incorporates both thermodynamic and kinetic considerations and allows going beyond the activity volcano model.
NI Journal Papers ; NI论文
NSFC of China["22102207","22022504"] ; Guangdong "Pearl River" Talent Plan[2019QN01L353] ; Shenzhen Science and Technology Program[JCYJ2021-03241036-08023] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]
|WOS Research Area|
|WOS Accession No|
Cited Times [WOS]:2
|Document Type||Journal Article|
|Department||Department of Chemistry|
1.Department of Chemistry,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
2.Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
3.School of Chemistry,Chemical Engineering and Biotechnology,Nanyang Technological University,Singapore,637459,Singapore
4.Department of Chemistry and Biochemistry,University of California,Los Angeles,90095,United States
5.Department of Materials Science and Engineering,City University of Hong Kong,999077,Hong Kong
6.Department of Chemistry,Tsinghua University,Beijing,100084,China
|First Author Affilication||Department of Chemistry; Southern University of Science and Technology|
|First Author's First Affilication||Department of Chemistry|
Cao，Hao,Wang，Qilun,Zhang，Zisheng,et al. Engineering Single-Atom Electrocatalysts for Enhancing Kinetics of Acidic Volmer Reaction[J]. Journal of the American Chemical Society,2023,145(24):13038-13047.
Cao，Hao.,Wang，Qilun.,Zhang，Zisheng.,Yan，Hui Min.,Zhao，Hongyan.,...&Wang，Yang Gang.(2023).Engineering Single-Atom Electrocatalysts for Enhancing Kinetics of Acidic Volmer Reaction.Journal of the American Chemical Society,145(24),13038-13047.
Cao，Hao,et al."Engineering Single-Atom Electrocatalysts for Enhancing Kinetics of Acidic Volmer Reaction".Journal of the American Chemical Society 145.24(2023):13038-13047.
|Files in This Item:||There are no files associated with this item.|
|Recommend this item|
|Export to Endnote|
|Export to Excel|
|Export to Csv|
|Similar articles in Google Scholar|
|Similar articles in Baidu Scholar|
|Similar articles in Bing Scholar|
Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.