Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Carbon doping switching on the hydrogen adsorption activity of NiO for hydrogen evolution reaction

Abstract

Hydrogen evolution reaction (HER) is more sluggish in alkaline than in acidic media because of the additional energy required for water dissociation. Numerous catalysts, including NiO, that offer active sites for water dissociation have been extensively investigated. Yet, the overall HER performance of NiO is still limited by lacking favorable H adsorption sites. Here we show a strategy to activate NiO through carbon doping, which creates under-coordinated Ni sites favorable for H adsorption. DFT calculations reveal that carbon dopant decreases the energy barrier of Heyrovsky step from 1.17 eV to 0.81 eV, suggesting the carbon also serves as a hot-spot for the dissociation of water molecules in water-alkali HER. As a result, the carbon doped NiO catalyst achieves an ultralow overpotential of 27 mV at 10 mA cm-2, and a low Tafel slope of 36 mV dec-1, representing the best performance among the state-of-the-art NiO catalysts.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [3];  [1];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [2];  [1];  [1]
+ Show Author Affiliations
  1. Univ. of California, Santa Cruz, CA (United States)
  2. Univ. of Science and Technology of China, Hefei (China)
  3. Shandong Univ., Jinan (China)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Aeronautics and Space Administration (NASA); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); National Key Research and Development Program of China; Natural Science Fund of China
OSTI Identifier:
1603613
Grant/Contract Number:  
AC02-05CH11231; SC0012704; ACI-1548562; AST 1828315; TG-DMR160105
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalyst synthesis; catalytic mechanisms; electrocatalysis

Citation Formats

Kou, Tianyi, Chen, Mingpeng, Wu, Feng, Smart, Tyler J., Wang, Shanwen, Wu, Yishang, Zhang, Ying, Li, Shengtong, Lall, Supriya, Zhang, Zhonghua, Liu, Yi-Sheng, Guo, Jinghua, Wang, Gongming, Ping, Yuan, and Li, Yat. Carbon doping switching on the hydrogen adsorption activity of NiO for hydrogen evolution reaction. United States: N. p., 2020. Web. doi:10.1038/s41467-020-14462-2.
Copy to clipboard
Kou, Tianyi, Chen, Mingpeng, Wu, Feng, Smart, Tyler J., Wang, Shanwen, Wu, Yishang, Zhang, Ying, Li, Shengtong, Lall, Supriya, Zhang, Zhonghua, Liu, Yi-Sheng, Guo, Jinghua, Wang, Gongming, Ping, Yuan, & Li, Yat. Carbon doping switching on the hydrogen adsorption activity of NiO for hydrogen evolution reaction. United States. https://doi.org/10.1038/s41467-020-14462-2
Copy to clipboard
Kou, Tianyi, Chen, Mingpeng, Wu, Feng, Smart, Tyler J., Wang, Shanwen, Wu, Yishang, Zhang, Ying, Li, Shengtong, Lall, Supriya, Zhang, Zhonghua, Liu, Yi-Sheng, Guo, Jinghua, Wang, Gongming, Ping, Yuan, and Li, Yat. Thu . "Carbon doping switching on the hydrogen adsorption activity of NiO for hydrogen evolution reaction". United States. https://doi.org/10.1038/s41467-020-14462-2. https://www.osti.gov/servlets/purl/1603613.
Copy to clipboard
@article{osti_1603613,
title = {Carbon doping switching on the hydrogen adsorption activity of NiO for hydrogen evolution reaction},
author = {Kou, Tianyi and Chen, Mingpeng and Wu, Feng and Smart, Tyler J. and Wang, Shanwen and Wu, Yishang and Zhang, Ying and Li, Shengtong and Lall, Supriya and Zhang, Zhonghua and Liu, Yi-Sheng and Guo, Jinghua and Wang, Gongming and Ping, Yuan and Li, Yat},
abstractNote = {Hydrogen evolution reaction (HER) is more sluggish in alkaline than in acidic media because of the additional energy required for water dissociation. Numerous catalysts, including NiO, that offer active sites for water dissociation have been extensively investigated. Yet, the overall HER performance of NiO is still limited by lacking favorable H adsorption sites. Here we show a strategy to activate NiO through carbon doping, which creates under-coordinated Ni sites favorable for H adsorption. DFT calculations reveal that carbon dopant decreases the energy barrier of Heyrovsky step from 1.17 eV to 0.81 eV, suggesting the carbon also serves as a hot-spot for the dissociation of water molecules in water-alkali HER. As a result, the carbon doped NiO catalyst achieves an ultralow overpotential of 27 mV at 10 mA cm-2, and a low Tafel slope of 36 mV dec-1, representing the best performance among the state-of-the-art NiO catalysts.},
doi = {10.1038/s41467-020-14462-2},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Thu Jan 30 00:00:00 EST 2020},
month = {Thu Jan 30 00:00:00 EST 2020}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-020-14462-2
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 121 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis
journal, April 2018

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Improved Electrochemical Phase Diagrams from Theory and Experiment: The Ni–Water System and Its Complex Compounds
journal, May 2017

  • Huang, L. -F.; Hutchison, M. J.; Santucci, R. J.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 18
  • DOI: 10.1021/acs.jpcc.7b02771

Trends in the Carbonyl Core (C 1S, O 1S) → π* C=O Transition in the Near-Edge X-ray Absorption Fine Structure Spectra of Organic Molecules
journal, August 2002

  • Urquhart, S. G.; Ade, H.
  • The Journal of Physical Chemistry B, Vol. 106, Issue 34
  • DOI: 10.1021/jp0255379

Carbon K -edge spectra of carbonate minerals
journal, July 2010

  • Brandes, Jay A.; Wirick, Sue; Jacobsen, Chris
  • Journal of Synchrotron Radiation, Vol. 17, Issue 5
  • DOI: 10.1107/S0909049510020029

Analysis of the Dissociation of H 2 O in Water Using First-Principles Molecular Dynamics
journal, August 1999

  • Trout, Bernhardt L.; Parrinello, Michele
  • The Journal of Physical Chemistry B, Vol. 103, Issue 34
  • DOI: 10.1021/jp990548w

The Reaction Mechanism with Free Energy Barriers at Constant Potentials for the Oxygen Evolution Reaction at the IrO 2 (110) Surface
journal, December 2016

  • Ping, Yuan; Nielsen, Robert J.; Goddard, William A.
  • Journal of the American Chemical Society, Vol. 139, Issue 1
  • DOI: 10.1021/jacs.6b07557

Blending Cr 2 O 3 into a NiO-Ni Electrocatalyst for Sustained Water Splitting
journal, August 2015

  • Gong, Ming; Zhou, Wu; Kenney, Michael James
  • Angewandte Chemie International Edition, Vol. 54, Issue 41
  • DOI: 10.1002/anie.201504815

Oxygen-Containing Functional Groups on Single-Wall Carbon Nanotubes:  NEXAFS and Vibrational Spectroscopic Studies
journal, October 2001

  • Kuznetsova, Anya; Popova, Irene; Yates, John T.
  • Journal of the American Chemical Society, Vol. 123, Issue 43
  • DOI: 10.1021/ja011021b

Study of Ni-Catalyzed Graphitization Process of Diamond by in Situ X-ray Photoelectron Spectroscopy
journal, March 2018

  • Romanyuk, O.; Varga, M.; Tulic, S.
  • The Journal of Physical Chemistry C, Vol. 122, Issue 12
  • DOI: 10.1021/acs.jpcc.7b12334

Theoretical and Experimental Insight into the Effect of Nitrogen Doping on Hydrogen Evolution Activity of Ni 3 S 2 in Alkaline Medium
journal, March 2018

Phonons and related crystal properties from density-functional perturbation theory
journal, July 2001

  • Baroni, Stefano; de Gironcoli, Stefano; Dal Corso, Andrea
  • Reviews of Modern Physics, Vol. 73, Issue 2
  • DOI: 10.1103/RevModPhys.73.515

Water Dissociative Adsorption on NiO(111): Energetics and Structure of the Hydroxylated Surface
journal, October 2016

Recent progress in alkaline water electrolysis for hydrogen production and applications
journal, June 2010

Understanding the Doping Effect on NiO: Toward High-Performance Inverted Perovskite Solar Cells
journal, March 2018

Doping high-surface-area mesoporous TiO 2 microspheres with carbonate for visible light hydrogen production
journal, January 2014

  • Liu, Bin; Liu, Li-Min; Lang, Xiu-Feng
  • Energy & Environmental Science, Vol. 7, Issue 8
  • DOI: 10.1039/C4EE00472H

Effect of Li doping in NiO thin films on its transparent and conducting properties and its application in heteroepitaxial p-n junctions
journal, October 2010

  • Dutta, Titas; Gupta, P.; Gupta, A.
  • Journal of Applied Physics, Vol. 108, Issue 8
  • DOI: 10.1063/1.3499276

Molecular adsorption on the surface of strongly correlated transition-metal oxides: A case study for CO/NiO(100)
journal, February 2004

NiO nanorod array anchored Ni foam as a binder-free anode for high-rate lithium ion batteries
journal, January 2014

  • Yang, Wanfeng; Cheng, Guanhua; Dong, Chaoqun
  • J. Mater. Chem. A, Vol. 2, Issue 47
  • DOI: 10.1039/C4TA04809A

Nanoscale nickel oxide/nickel heterostructures for active hydrogen evolution electrocatalysis
journal, August 2014

  • Gong, Ming; Zhou, Wu; Tsai, Mon-Che
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5695

The importance of nonlinear fluid response in joint density-functional theory studies of battery systems
journal, October 2013

  • Gunceler, Deniz; Letchworth-Weaver, Kendra; Sundararaman, Ravishankar
  • Modelling and Simulation in Materials Science and Engineering, Vol. 21, Issue 7
  • DOI: 10.1088/0965-0393/21/7/074005

Carbon Nitride Deposited Using Energetic Species: A Two-Phase System
journal, July 1994

A fast and robust algorithm for Bader decomposition of charge density
journal, June 2006

Ni Foam-Supported Fe-Doped β-Ni(OH) 2 Nanosheets Show Ultralow Overpotential for Oxygen Evolution Reaction
journal, January 2019

Engineering oxygen vacancy on NiO nanorod arrays for alkaline hydrogen evolution
journal, January 2018

Progress in understanding hematite electrochemistry through computational modeling
journal, April 2019

Electronic and transport properties of Li-doped NiO epitaxial thin films
journal, January 2018

  • Zhang, J. Y.; Li, W. W.; Hoye, R. L. Z.
  • Journal of Materials Chemistry C, Vol. 6, Issue 9
  • DOI: 10.1039/C7TC05331B

Dominating Role of Ni 0 on the Interface of Ni/NiO for Enhanced Hydrogen Evolution Reaction
journal, February 2017

  • Wang, Jing; Mao, Shanjun; Liu, Zeyan
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 8
  • DOI: 10.1021/acsami.6b15377

X-ray photoelectron spectra of defective nickel oxide
journal, January 1988

  • Tomellini, Massimo
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 84, Issue 10
  • DOI: 10.1039/f19888403501

Efficient Metal-Free Electrocatalysts for Oxygen Reduction: Polyaniline-Derived N- and O-Doped Mesoporous Carbons
journal, May 2013

  • Silva, Rafael; Voiry, Damien; Chhowalla, Manish
  • Journal of the American Chemical Society, Vol. 135, Issue 21
  • DOI: 10.1021/ja402450a

A dimer method for finding saddle points on high dimensional potential surfaces using only first derivatives
journal, October 1999

  • Henkelman, Graeme; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 111, Issue 15
  • DOI: 10.1063/1.480097

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

  • Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
  • DOI: 10.1063/1.1329672

Nanostructured mesoporous nickel oxide thin films
journal, February 2007

Accounting for Nanometer-Thick Adventitious Carbon Contamination in X-ray Absorption Spectra of Carbon-Based Materials
journal, November 2014

  • Mangolini, Filippo; McClimon, J. Brandon; Rose, Franck
  • Analytical Chemistry, Vol. 86, Issue 24
  • DOI: 10.1021/ac503409c

Ferromagnetic dislocations in antiferromagnetic NiO
journal, March 2013

  • Sugiyama, Issei; Shibata, Naoya; Wang, Zhongchang
  • Nature Nanotechnology, Vol. 8, Issue 4
  • DOI: 10.1038/nnano.2013.45

Stability of the polar NiO(111) surface
journal, March 2008

  • Zhang, Wei-Bing; Tang, Bi-Yu
  • The Journal of Chemical Physics, Vol. 128, Issue 12
  • DOI: 10.1063/1.2835544

A mini review on nickel-based electrocatalysts for alkaline hydrogen evolution reaction
journal, December 2015

Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes
journal, January 2010

  • Sheng, Wenchao; Gasteiger, Hubert A.; Shao-Horn, Yang
  • Journal of The Electrochemical Society, Vol. 157, Issue 11
  • DOI: 10.1149/1.3483106

New interpretations of XPS spectra of nickel metal and oxides
journal, May 2006

  • Grosvenor, Andrew P.; Biesinger, Mark C.; Smart, Roger St. C.
  • Surface Science, Vol. 600, Issue 9
  • DOI: 10.1016/j.susc.2006.01.041

Pseudopotentials for high-throughput DFT calculations
journal, January 2014

Crystalline/amorphous Ni/NiO core/shell nanosheets as highly active electrocatalysts for hydrogen evolution reaction
journal, December 2015

Non-Noble Metal-based Carbon Composites in Hydrogen Evolution Reaction: Fundamentals to Applications
journal, February 2017

The importance of nonlinear fluid response in joint density-functional theory studies of battery systems
text, January 2013

Pseudopotentials for high-throughput DFT calculations
text, January 2013

Blending Cr 2 O 3 into a NiO-Ni Electrocatalyst for Sustained Water Splitting
journal, August 2015

  • Gong, Ming; Zhou, Wu; Kenney, Michael James
  • Angewandte Chemie International Edition, Vol. 54, Issue 41
  • DOI: 10.1002/anie.201504815

Bioinformatics and metabolic flux analysis highlight a new mechanism involved in lactate oxidation in Clostridium tyrobutyricum
journal, January 2023

A mini review on nickel-based electrocatalysts for alkaline hydrogen evolution reaction
journal, December 2015

Engineering oxygen vacancy on NiO nanorod arrays for alkaline hydrogen evolution
journal, January 2018

New interpretations of XPS spectra of nickel metal and oxides
journal, May 2006

  • Grosvenor, Andrew P.; Biesinger, Mark C.; Smart, Roger St. C.
  • Surface Science, Vol. 600, Issue 9
  • DOI: 10.1016/j.susc.2006.01.041

Accounting for Nanometer-Thick Adventitious Carbon Contamination in X-ray Absorption Spectra of Carbon-Based Materials
journal, November 2014

  • Mangolini, Filippo; McClimon, J. Brandon; Rose, Franck
  • Analytical Chemistry, Vol. 86, Issue 24
  • DOI: 10.1021/ac503409c

Improved Electrochemical Phase Diagrams from Theory and Experiment: The Ni–Water System and Its Complex Compounds
journal, May 2017

  • Huang, L. -F.; Hutchison, M. J.; Santucci, R. J.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 18
  • DOI: 10.1021/acs.jpcc.7b02771

Water Dissociative Adsorption on NiO(111): Energetics and Structure of the Hydroxylated Surface
journal, October 2016

Oxygen-Containing Functional Groups on Single-Wall Carbon Nanotubes:  NEXAFS and Vibrational Spectroscopic Studies
journal, October 2001

  • Kuznetsova, Anya; Popova, Irene; Yates, John T.
  • Journal of the American Chemical Society, Vol. 123, Issue 43
  • DOI: 10.1021/ja011021b

Efficient Metal-Free Electrocatalysts for Oxygen Reduction: Polyaniline-Derived N- and O-Doped Mesoporous Carbons
journal, May 2013

  • Silva, Rafael; Voiry, Damien; Chhowalla, Manish
  • Journal of the American Chemical Society, Vol. 135, Issue 21
  • DOI: 10.1021/ja402450a

The Reaction Mechanism with Free Energy Barriers at Constant Potentials for the Oxygen Evolution Reaction at the IrO 2 (110) Surface
journal, December 2016

  • Ping, Yuan; Nielsen, Robert J.; Goddard, William A.
  • Journal of the American Chemical Society, Vol. 139, Issue 1
  • DOI: 10.1021/jacs.6b07557

Analysis of the Dissociation of H 2 O in Water Using First-Principles Molecular Dynamics
journal, August 1999

  • Trout, Bernhardt L.; Parrinello, Michele
  • The Journal of Physical Chemistry B, Vol. 103, Issue 34
  • DOI: 10.1021/jp990548w

Nanoscale nickel oxide/nickel heterostructures for active hydrogen evolution electrocatalysis
journal, August 2014

  • Gong, Ming; Zhou, Wu; Tsai, Mon-Che
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5695

Ferromagnetic dislocations in antiferromagnetic NiO
journal, March 2013

  • Sugiyama, Issei; Shibata, Naoya; Wang, Zhongchang
  • Nature Nanotechnology, Vol. 8, Issue 4
  • DOI: 10.1038/nnano.2013.45

Structural dynamics of basaltic melt at mantle conditions with implications for magma oceans and superplumes
journal, September 2020

X-ray photoelectron spectra of defective nickel oxide
journal, January 1988

  • Tomellini, Massimo
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 84, Issue 10
  • DOI: 10.1039/f19888403501

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

  • Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
  • DOI: 10.1063/1.1329672

Stability of the polar NiO(111) surface
journal, March 2008

  • Zhang, Wei-Bing; Tang, Bi-Yu
  • The Journal of Chemical Physics, Vol. 128, Issue 12
  • DOI: 10.1063/1.2835544

A dimer method for finding saddle points on high dimensional potential surfaces using only first derivatives
journal, October 1999

  • Henkelman, Graeme; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 111, Issue 15
  • DOI: 10.1063/1.480097

Nanostructured mesoporous nickel oxide thin films
journal, February 2007

Path-integral simulation of positronium in a hard sphere
journal, July 1989

Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes
journal, January 2010

  • Sheng, Wenchao; Gasteiger, Hubert A.; Shao-Horn, Yang
  • Journal of The Electrochemical Society, Vol. 157, Issue 11
  • DOI: 10.1149/1.3483106

Pseudopotentials for high-throughput DFT calculations
text, January 2013

    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: