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Title: Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction

Abstract

The proper choice of nonprecious transition metals as single atom catalysts (SACs) remains unclear for designing highly efficient electrocatalysts for hydrogen evolution reaction (HER). Herein, reported is an activity correlation with catalysts, electronic structure, in order to clarify the origin of reactivity for a series of transition metals supported on nitrogen-doped graphene as SACs for HER by a combination of density functional theory calculations and electrochemical measurements. Only few of the transition metals (e.g., Co, Cr, Fe, Rh, and V) as SACs show good catalytic activity toward HER as their Gibbs free energies are varied between the range of -0.20 to 0.30 eV but among which Co-SAC exhibits the highest electrochemical activity at 0.13 eV. Electronic structure studies show that the energy states of active valence d(z)(2) orbitals and their resulting antibonding state determine the catalytic activity for HER. The fact that the antibonding state orbital is neither completely empty nor fully filled in the case of Co-SAC is the main reason for its ideal hydrogen adsorption energy. Moreover, the electrochemical measurement shows that Co-SAC exhibits a superior hydrogen evolution activity over Ni-SAC and W-SAC, confirming the theoretical calculation. This systematic study gives a fundamental understanding about the design ofmore » highly efficient SACs for HER.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [1];  [1];  [5];  [1];  [6];  [7];  [8];  [3]; ORCiD logo [1]
  1. Department of Chemical and Biological Engineering, William Mong Institute of Nano Science and Technology, and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology, Clear Water Bay Kowloon 999077 Hong Kong
  2. Department of Materials Science and Engineering, University of California-Irvine, Irvine CA 92697 USA
  3. Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue Lemont IL 60439 USA
  4. Department of Physics and Astronomy, University of California-Irvine, Irvine CA 92697 USA
  5. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue Lemont IL 60439 USA
  6. The Smart Materials Research Institute, Southern Federal University, 344090 Rostov-on-Don Russia
  7. National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Collaborative Innovation Center of Advanced Microstructures, and Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing 210093 China
  8. Department of Materials Science and Engineering, University of California-Irvine, Irvine CA 92697 USA; Department of Physics and Astronomy, University of California-Irvine, Irvine CA 92697 USA
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Office of Vehicle Technology - Battery Materials Research (BMR) Program; National Natural Science Foundation of China (NNSFC); Research Grants Council (RGC) of Hong Kong; Southern Federal University; Hong Kong University of Science and Technology (HKUST); USDOE
OSTI Identifier:
1502877
Alternate Identifier(s):
OSTI ID: 1492093
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 10; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
charge transfer; density functional theory; density of states; hydrogen evolution reaction; single atom catalysts

Citation Formats

Hossain, Md Delowar, Liu, Zhenjing, Zhuang, Minghao, Yan, Xingxu, Xu, Gui-Liang, Gadre, Chaitanya Avinash, Tyagi, Abhishek, Abidi, Irfan Haider, Sun, Cheng-Jun, Wong, Hoilun, Guda, Alexander, Hao, Yufeng, Pan, Xiaoqing, Amine, Khalil, and Luo, Zhengtang. Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction. United States: N. p., 2019. Web. doi:10.1002/aenm.201803689.
Hossain, Md Delowar, Liu, Zhenjing, Zhuang, Minghao, Yan, Xingxu, Xu, Gui-Liang, Gadre, Chaitanya Avinash, Tyagi, Abhishek, Abidi, Irfan Haider, Sun, Cheng-Jun, Wong, Hoilun, Guda, Alexander, Hao, Yufeng, Pan, Xiaoqing, Amine, Khalil, & Luo, Zhengtang. Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction. United States. doi:10.1002/aenm.201803689.
Hossain, Md Delowar, Liu, Zhenjing, Zhuang, Minghao, Yan, Xingxu, Xu, Gui-Liang, Gadre, Chaitanya Avinash, Tyagi, Abhishek, Abidi, Irfan Haider, Sun, Cheng-Jun, Wong, Hoilun, Guda, Alexander, Hao, Yufeng, Pan, Xiaoqing, Amine, Khalil, and Luo, Zhengtang. Fri . "Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction". United States. doi:10.1002/aenm.201803689.
@article{osti_1502877,
title = {Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction},
author = {Hossain, Md Delowar and Liu, Zhenjing and Zhuang, Minghao and Yan, Xingxu and Xu, Gui-Liang and Gadre, Chaitanya Avinash and Tyagi, Abhishek and Abidi, Irfan Haider and Sun, Cheng-Jun and Wong, Hoilun and Guda, Alexander and Hao, Yufeng and Pan, Xiaoqing and Amine, Khalil and Luo, Zhengtang},
abstractNote = {The proper choice of nonprecious transition metals as single atom catalysts (SACs) remains unclear for designing highly efficient electrocatalysts for hydrogen evolution reaction (HER). Herein, reported is an activity correlation with catalysts, electronic structure, in order to clarify the origin of reactivity for a series of transition metals supported on nitrogen-doped graphene as SACs for HER by a combination of density functional theory calculations and electrochemical measurements. Only few of the transition metals (e.g., Co, Cr, Fe, Rh, and V) as SACs show good catalytic activity toward HER as their Gibbs free energies are varied between the range of -0.20 to 0.30 eV but among which Co-SAC exhibits the highest electrochemical activity at 0.13 eV. Electronic structure studies show that the energy states of active valence d(z)(2) orbitals and their resulting antibonding state determine the catalytic activity for HER. The fact that the antibonding state orbital is neither completely empty nor fully filled in the case of Co-SAC is the main reason for its ideal hydrogen adsorption energy. Moreover, the electrochemical measurement shows that Co-SAC exhibits a superior hydrogen evolution activity over Ni-SAC and W-SAC, confirming the theoretical calculation. This systematic study gives a fundamental understanding about the design of highly efficient SACs for HER.},
doi = {10.1002/aenm.201803689},
journal = {Advanced Energy Materials},
issn = {1614-6832},
number = 10,
volume = 9,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
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