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

Title: Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis

Abstract

The grand challenge in the development of atomically dispersed metallic catalysts is their low metal-atom loading density, uncontrollable localization and ambiguous interactions with supports, posing difficulty in maximizing their catalytic performance. Here, we achieve an interface catalyst consisting of atomic cobalt array covalently bound to distorted 1T MoS2 nanosheets (SA Co-D 1T MoS2). The phase of MoS2 transforming from 2H to D-1T, induced by strain from lattice mismatch and formation of Co-S covalent bond between Co and MoS2 during the assembly, is found to be essential to form the highly active single-atom array catalyst. SA Co-D 1T MoS2 achieves Pt-like activity toward HER and high long-term stability. Active-site blocking experiment together with density functional theory (DFT) calculations reveal that the superior catalytic behaviour is associated with an ensemble effect via the synergy of Co adatom and S of the D-1T MoS2 support by tuning hydrogen binding mode at the interface.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1];  [3];  [1];  [1];  [2];  [2];  [4];  [2];  [3];  [3];  [1];  [1]; ORCiD logo [3];  [1]; ORCiD logo [5]
+ Show Author Affiliations
  1. Jilin Univ., Changchun (China)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Peking Univ., Beijing (China)
  4. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Applied Physics, Shanghai Synchrotron Radiation Facility
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1579497
Report Number(s):
BNL-212407-2019-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; 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

Citation Formats

Qi, Kun, Cui, Xiaoqiang, Gu, Lin, Yu, Shansheng, Fan, Xiaofeng, Luo, Mingchuan, Xu, Shan, Li, Ningbo, Zheng, Lirong, Zhang, Qinghua, Ma, Jingyuan, Gong, Yue, Lv, Fan, Wang, Kai, Huang, Haihua, Zhang, Wei, Guo, Shaojun, Zheng, Weitao, and Liu, Ping. Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis. United States: N. p., 2019. Web. doi:10.1038/s41467-019-12997-7.
Copy to clipboard
Qi, Kun, Cui, Xiaoqiang, Gu, Lin, Yu, Shansheng, Fan, Xiaofeng, Luo, Mingchuan, Xu, Shan, Li, Ningbo, Zheng, Lirong, Zhang, Qinghua, Ma, Jingyuan, Gong, Yue, Lv, Fan, Wang, Kai, Huang, Haihua, Zhang, Wei, Guo, Shaojun, Zheng, Weitao, & Liu, Ping. Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis. United States. https://doi.org/10.1038/s41467-019-12997-7
Copy to clipboard
Qi, Kun, Cui, Xiaoqiang, Gu, Lin, Yu, Shansheng, Fan, Xiaofeng, Luo, Mingchuan, Xu, Shan, Li, Ningbo, Zheng, Lirong, Zhang, Qinghua, Ma, Jingyuan, Gong, Yue, Lv, Fan, Wang, Kai, Huang, Haihua, Zhang, Wei, Guo, Shaojun, Zheng, Weitao, and Liu, Ping. Tue . "Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis". United States. https://doi.org/10.1038/s41467-019-12997-7. https://www.osti.gov/servlets/purl/1579497.
Copy to clipboard
@article{osti_1579497,
title = {Single-atom cobalt array bound to distorted 1T MoS2 with ensemble effect for hydrogen evolution catalysis},
author = {Qi, Kun and Cui, Xiaoqiang and Gu, Lin and Yu, Shansheng and Fan, Xiaofeng and Luo, Mingchuan and Xu, Shan and Li, Ningbo and Zheng, Lirong and Zhang, Qinghua and Ma, Jingyuan and Gong, Yue and Lv, Fan and Wang, Kai and Huang, Haihua and Zhang, Wei and Guo, Shaojun and Zheng, Weitao and Liu, Ping},
abstractNote = {The grand challenge in the development of atomically dispersed metallic catalysts is their low metal-atom loading density, uncontrollable localization and ambiguous interactions with supports, posing difficulty in maximizing their catalytic performance. Here, we achieve an interface catalyst consisting of atomic cobalt array covalently bound to distorted 1T MoS2 nanosheets (SA Co-D 1T MoS2). The phase of MoS2 transforming from 2H to D-1T, induced by strain from lattice mismatch and formation of Co-S covalent bond between Co and MoS2 during the assembly, is found to be essential to form the highly active single-atom array catalyst. SA Co-D 1T MoS2 achieves Pt-like activity toward HER and high long-term stability. Active-site blocking experiment together with density functional theory (DFT) calculations reveal that the superior catalytic behaviour is associated with an ensemble effect via the synergy of Co adatom and S of the D-1T MoS2 support by tuning hydrogen binding mode at the interface.},
doi = {10.1038/s41467-019-12997-7},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Tue Nov 19 00:00:00 EST 2019},
month = {Tue Nov 19 00:00:00 EST 2019}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-019-12997-7
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 271 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:

Low-dimensional catalysts for hydrogen evolution and CO2 reduction
journal, January 2018

  • Voiry, Damien; Shin, Hyeon Suk; Loh, Kian Ping
  • Nature Reviews Chemistry, Vol. 2, Issue 1
  • DOI: 10.1038/s41570-017-0105

Efficient hydrogen evolution catalysis using ternary pyrite-type cobalt phosphosulphide
journal, September 2015

  • Cabán-Acevedo, Miguel; Stone, Michael L.; Schmidt, J. R.
  • Nature Materials, Vol. 14, Issue 12
  • DOI: 10.1038/nmat4410

Combining theory and experiment in electrocatalysis: Insights into materials design
journal, January 2017

MoS2 Nanoparticles Grown on Graphene An Advanced Catalyst for the Hydrogen Evolution Reaction
journal, May 2011

  • Li, Yanguang; Wang, Hailiang; Xie, Liming
  • Journal of the American Chemical Society, Vol. 133, Issue 19, p. 7296-7299
  • DOI: 10.1021/ja201269b

Noble metal-free hydrogen evolution catalysts for water splitting
journal, January 2015

  • Zou, Xiaoxin; Zhang, Yu
  • Chemical Society Reviews, Vol. 44, Issue 15
  • DOI: 10.1039/C4CS00448E

Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts
journal, July 2007

  • Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J.
  • Science, Vol. 317, Issue 5834, p. 100-102
  • DOI: 10.1126/science.1141483

Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies
journal, November 2015

  • Li, Hong; Tsai, Charlie; Koh, Ai Leen
  • Nature Materials, Vol. 15, Issue 1
  • DOI: 10.1038/nmat4465

Photochemical route for synthesizing atomically dispersed palladium catalysts
journal, May 2016

Anchoring zero valence single atoms of nickel and iron on graphdiyne for hydrogen evolution
journal, April 2018

Synergetic interaction between neighbouring platinum monomers in CO2 hydrogenation
journal, March 2018

A universal principle for a rational design of single-atom electrocatalysts
journal, April 2018

Heterogeneous single-atom catalysis
journal, May 2018

Single-Atom Electrocatalysts
journal, October 2017

  • Zhu, Chengzhou; Fu, Shaofang; Shi, Qiurong
  • Angewandte Chemie International Edition, Vol. 56, Issue 45
  • DOI: 10.1002/anie.201703864

The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen
journal, June 2016

  • Voiry, Damien; Fullon, Raymond; Yang, Jieun
  • Nature Materials, Vol. 15, Issue 9
  • DOI: 10.1038/nmat4660

Interaction trends between single metal atoms and oxide supports identified with density functional theory and statistical learning
journal, July 2018

  • O’Connor, Nolan J.; Jonayat, A. S. M.; Janik, Michael J.
  • Nature Catalysis, Vol. 1, Issue 7
  • DOI: 10.1038/s41929-018-0094-5

Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2
journal, April 2014

  • Lin, Yung-Chang; Dumcenco, Dumitru O.; Huang, Ying-Sheng
  • Nature Nanotechnology, Vol. 9, Issue 5
  • DOI: 10.1038/nnano.2014.64

Design of active and stable Co–Mo–Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction
journal, November 2015

  • Staszak-Jirkovský, Jakub; Malliakas, Christos D.; Lopes, Pietro P.
  • Nature Materials, Vol. 15, Issue 2
  • DOI: 10.1038/nmat4481

Spin-Dependent Tunneling in Self-Assembled Cobalt-Nanocrystal Superlattices
journal, November 2000

Metallic Contact between MoS 2 and Ni via Au Nanoglue
journal, April 2018

Atomically isolated nickel species anchored on graphitized carbon for efficient hydrogen evolution electrocatalysis
journal, February 2016

  • Fan, Lili; Liu, Peng Fei; Yan, Xuecheng
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10667

High-performance hybrid oxide catalyst of manganese and cobalt for low-pressure methanol synthesis
journal, March 2015

  • Li, Cheng-Shiuan; Melaet, Gérôme; Ralston, Walter T.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7538

Single-atom cobalt electrocatalysts for foldable solid-state Zn-air battery
journal, August 2018

Operando Spectroscopic Analysis of an Amorphous Cobalt Sulfide Hydrogen Evolution Electrocatalyst
journal, June 2015

  • Kornienko, Nikolay; Resasco, Joaquin; Becknell, Nigel
  • Journal of the American Chemical Society, Vol. 137, Issue 23
  • DOI: 10.1021/jacs.5b03545

Design of Single-Atom Co–N 5 Catalytic Site: A Robust Electrocatalyst for CO 2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability
journal, February 2018

  • Pan, Yuan; Lin, Rui; Chen, Yinjuan
  • Journal of the American Chemical Society, Vol. 140, Issue 12
  • DOI: 10.1021/jacs.8b00814

X-ray electron density investigation of chemical bonding in van der Waals materials
journal, February 2018

Single-atom dispersed Co–N–C catalyst: structure identification and performance for hydrogenative coupling of nitroarenes
journal, January 2016

  • Liu, Wengang; Zhang, Leilei; Yan, Wensheng
  • Chemical Science, Vol. 7, Issue 9
  • DOI: 10.1039/C6SC02105K

High phase-purity 1T′-MoS2- and 1T′-MoSe2-layered crystals
journal, April 2018

Vacancy-Induced Ferromagnetism of MoS 2 Nanosheets
journal, February 2015

  • Cai, Liang; He, Jingfu; Liu, Qinghua
  • Journal of the American Chemical Society, Vol. 137, Issue 7
  • DOI: 10.1021/ja5120908

Multiscale structural and electronic control of molybdenum disulfide foam for highly efficient hydrogen production
journal, April 2017

  • Deng, Jiao; Li, Haobo; Wang, Suheng
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14430

Preparation of Single-Layer MoS 2 x Se 2(1- x ) and Mo x W 1- x S 2 Nanosheets with High-Concentration Metallic 1T Phase
journal, February 2016

Room Temperature Semiconductor–Metal Transition of MoTe 2 Thin Films Engineered by Strain
journal, December 2015

Amorphous MoS x Cl y electrocatalyst supported by vertical graphene for efficient electrochemical and photoelectrochemical hydrogen generation
journal, January 2015

  • Zhang, Xingwang; Meng, Fei; Mao, Shun
  • Energy & Environmental Science, Vol. 8, Issue 3
  • DOI: 10.1039/C4EE03240C

Use of Platinum as the Counter Electrode to Study the Activity of Nonprecious Metal Catalysts for the Hydrogen Evolution Reaction
journal, April 2017

Molecular metal–Nx centres in porous carbon for electrocatalytic hydrogen evolution
journal, August 2015

  • Liang, Hai-Wei; Brüller, Sebastian; Dong, Renhao
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8992

Pure and stable metallic phase molybdenum disulfide nanosheets for hydrogen evolution reaction
journal, February 2016

  • Geng, Xiumei; Sun, Weiwei; Wu, Wei
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10672

Phenylenediamine-Based FeN x /C Catalyst with High Activity for Oxygen Reduction in Acid Medium and Its Active-Site Probing
journal, July 2014

  • Wang, Qiang; Zhou, Zhi-You; Lai, Yu-Jiao
  • Journal of the American Chemical Society, Vol. 136, Issue 31
  • DOI: 10.1021/ja505777v

Bonded-atom fragments for describing molecular charge densities
journal, January 1977

Defect-Rich MoS 2 Ultrathin Nanosheets with Additional Active Edge Sites for Enhanced Electrocatalytic Hydrogen Evolution
journal, August 2013

Solution synthesis of triangular and hexagonal nickel nanosheets with the aid of tungsten hexacarbonyl
journal, January 2016

  • Wang, Zhichao; Chen, Yuanzhi; Zeng, Deqian
  • CrystEngComm, Vol. 18, Issue 8
  • DOI: 10.1039/C5CE02187A

Comparison of Cobalt-based Nanoparticles as Electrocatalysts for Water Oxidation
journal, October 2011

Solution-phase epitaxial growth of noble metal nanostructures on dispersible single-layer molybdenum disulfide nanosheets
journal, February 2013

  • Huang, Xiao; Zeng, Zhiyuan; Bao, Shuyu
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2472

Triggering the electrocatalytic hydrogen evolution activity of the inert two-dimensional MoS 2 surface via single-atom metal doping
journal, January 2015

  • Deng, Jiao; Li, Haobo; Xiao, Jianping
  • Energy & Environmental Science, Vol. 8, Issue 5
  • DOI: 10.1039/C5EE00751H

Theoretical approaches to x-ray absorption fine structure
journal, July 2000

Revisiting the surface properties of Mg(0001) thin films and their effect on the adatom binding energy and self-diffusion
journal, February 2015

Characterization of bismuth–cerium-molybdate selective propylene ammoxidation catalysts
journal, April 2015

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

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

An all‐electron numerical method for solving the local density functional for polyatomic molecules
journal, January 1990

  • Delley, B.
  • The Journal of Chemical Physics, Vol. 92, Issue 1
  • DOI: 10.1063/1.458452

Azobenzene at coinage metal surfaces: Role of dispersive van der Waals interactions
journal, November 2009

Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

High-resolution X-ray luminescence extension imaging
journal, February 2021

Computational exploration of copper catalyzed vinylogous aerobic oxidation of unsaturated compounds
journal, January 2021

    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: