Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction

Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study...

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Published inNature communications Vol. 13; no. 1; pp. 6875 - 14
Main Authors Zhang, Tianyu, Jin, Jing, Chen, Junmei, Fang, Yingyan, Han, Xu, Chen, Jiayi, Li, Yaping, Wang, Yu, Liu, Junfeng, Wang, Lei
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 12.11.2022
Nature Publishing Group
Nature Portfolio
Subjects
119/118
140/131
140/133
140/146
147/135
147/137
147/143
639/301/299/886
639/638/675
639/925/357
Affinity
Alkaline water
Catalysis
Catalysts
Catalytic activity
Correlation
Electron affinity
Energy efficiency
Green hydrogen
Homogeneity
Humanities and Social Sciences
Hydrogen
Hydrogen evolution reactions
Iron compounds
Irradiation
Ligands
multidisciplinary
Nickel compounds
Platinum
Science
Science (multidisciplinary)
Single atom catalysts
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Abstract Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt −1 and turnover frequency of 30.3  H 2 s −1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions. Establishing robust structure/performance correlations is critical for the development of single-atom-catalysts with improved activity. Here, the axial ligand on Pt single-atom-catalyst is precisely adjusted and studied, showing that the ligand’s first electron affinity is crucial for the catalysis.
AbstractList Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt −1 and turnover frequency of 30.3  H 2 s −1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions. Establishing robust structure/performance correlations is critical for the development of single-atom-catalysts with improved activity. Here, the axial ligand on Pt single-atom-catalyst is precisely adjusted and studied, showing that the ligand’s first electron affinity is crucial for the catalysis.
Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (-F, -Cl, -Br, -I, -OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt-1 and turnover frequency of 30.3  H2 s-1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions.Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (-F, -Cl, -Br, -I, -OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt-1 and turnover frequency of 30.3  H2 s-1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions.
Establishing robust structure/performance correlations is critical for the development of single-atom-catalysts with improved activity. Here, the axial ligand on Pt single-atom-catalyst is precisely adjusted and studied, showing that the ligand’s first electron affinity is crucial for the catalysis.
Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt−1 and turnover frequency of 30.3  H2 s−1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions.Establishing robust structure/performance correlations is critical for the development of single-atom-catalysts with improved activity. Here, the axial ligand on Pt single-atom-catalyst is precisely adjusted and studied, showing that the ligand’s first electron affinity is crucial for the catalysis.
Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt −1 and turnover frequency of 30.3  H 2 s −1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions.
ArticleNumber 6875
Author Chen, Jiayi
Wang, Yu
Fang, Yingyan
Jin, Jing
Wang, Lei
Liu, Junfeng
Zhang, Tianyu
Chen, Junmei
Han, Xu
Li, Yaping
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  organization: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Department of Chemical and Biomolecular Engineering, National University of Singapore
– sequence: 2
  givenname: Jing
  surname: Jin
  fullname: Jin, Jing
  organization: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, State Key Laboratory of Acoustics, Institute of Acoustics, Chinese Academy of Sciences Institution
– sequence: 3
  givenname: Junmei
  surname: Chen
  fullname: Chen, Junmei
  organization: Department of Chemical and Biomolecular Engineering, National University of Singapore
– sequence: 4
  givenname: Yingyan
  surname: Fang
  fullname: Fang, Yingyan
  organization: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
– sequence: 5
  givenname: Xu
  surname: Han
  fullname: Han, Xu
  organization: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
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  fullname: Chen, Jiayi
  organization: Department of Chemical and Biomolecular Engineering, National University of Singapore
– sequence: 7
  givenname: Yaping
  surname: Li
  fullname: Li, Yaping
  organization: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
– sequence: 8
  givenname: Yu
  orcidid: 0000-0002-9071-0238
  surname: Wang
  fullname: Wang, Yu
  organization: Shanghai Synchrotron Radiation Facility, Zhangjiang Laboratory, Shanghai Advanced Research Institute, Chinese Academy of Sciences
– sequence: 9
  givenname: Junfeng
  orcidid: 0000-0002-7455-6314
  surname: Liu
  fullname: Liu, Junfeng
  email: ljf@mail.buct.edu.cn
  organization: State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology
– sequence: 10
  givenname: Lei
  orcidid: 0000-0002-1931-7767
  surname: Wang
  fullname: Wang, Lei
  email: wanglei8@nus.edu.sg
  organization: Department of Chemical and Biomolecular Engineering, National University of Singapore
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Snippet Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However,...
Establishing robust structure/performance correlations is critical for the development of single-atom-catalysts with improved activity. Here, the axial ligand...
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140/131
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639/638/675
639/925/357
Affinity
Alkaline water
Catalysis
Catalysts
Catalytic activity
Correlation
Electron affinity
Energy efficiency
Green hydrogen
Homogeneity
Humanities and Social Sciences
Hydrogen
Hydrogen evolution reactions
Iron compounds
Irradiation
Ligands
multidisciplinary
Nickel compounds
Platinum
Science
Science (multidisciplinary)
Single atom catalysts
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Title Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction
URI https://link.springer.com/article/10.1038/s41467-022-34619-5
https://www.proquest.com/docview/2735576597
https://www.proquest.com/docview/2735869550
https://pubmed.ncbi.nlm.nih.gov/PMC9653394
https://doaj.org/article/0c23a79eedd8437db06e78dfc0fffc68
Volume 13
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