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  Toward Activity Origin of Electrocatalytic Hydrogen Evolution Reaction on Carbon-Rich Crystalline Coordination Polymers

Wang, L., Tranca, D. C., Zhang, J., Qi, Y., Sfaelou, S., Zhang, T., et al. (2017). Toward Activity Origin of Electrocatalytic Hydrogen Evolution Reaction on Carbon-Rich Crystalline Coordination Polymers. Small, 13(37): 1700783, pp. 1-8. doi:10.1002/smll.201700783.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002E-1300-E Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002E-1322-2
Genre: Journal Article

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 Creators:
Wang, Lihuan1, Author
Tranca, Diana C.1, Author
Zhang, Jian1, Author
Qi, Yanpeng2, Author              
Sfaelou, Stavroula1, Author
Zhang, Tao1, Author
Dong, Renhao1, Author
Zhuang, Xiaodong1, Author
Zheng, Zhikun1, Author
Seifert, Gotthard1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863425              

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 Abstract: The fundamental understanding of electrocatalytic active sites for hydrogen evolution reaction (HER) is significantly important for the development of metal complex involved carbon electrocatalysts with low kinetic barrier. Here, the MSxNy (M = Fe, Co, and Ni, x/y are 2/2, 0/4, and 4/0, respectively) active centers are immobilized into ladder-type, highly crystalline coordination polymers as model carbon-rich electrocatalysts for H-2 generation in acid solution. The electrocatalytic HER tests reveal that the coordination of metal, sulfur, and nitrogen synergistically facilitates the hydrogen ad-/desorption on MSxNy catalysts, leading to enhanced HER kinetics. Toward the activity origin of MS2N2, the experimental and theoretical results disclose that the metal atoms are preferentially protonated and then the production of H-2 is favored on the MN active sites after a heterocoupling step involving a N-bound proton and a metal-bound hydride. Moreover, the tuning of the metal centers in MS2N2 leads to the HER performance in the order of FeS2N2 > CoS2N2 > NiS2N2. Thus, the understanding of the catalytic active sites provides strategies for the enhancement of the electrocatalytic activity by tailoring the ligands and metal centers to the desired function.

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Language(s): eng - English
 Dates: 2017-07-252017-07-25
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Method: -
 Identifiers: ISI: 000412167100014
DOI: 10.1002/smll.201700783
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Title: Small
  Other : Small
Source Genre: Journal
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Publ. Info: Weinheim, Germany : Wiley
Pages: - Volume / Issue: 13 (37) Sequence Number: 1700783 Start / End Page: 1 - 8 Identifier: ISSN: 1613-6810
CoNE: /journals/resource/1000000000017440_1