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Title: Nitrogen-doped tungsten carbide nanoarray as an efficient bifunctional electrocatalyst for water splitting in acid

Abstract

Tungsten carbide is one of the most promising electrocatalysts for the hydrogen evolution reaction, although it exhibits sluggish kinetics due to a strong tungsten-hydrogen bond. In addition, tungsten carbide’s catalytic activity toward the oxygen evolution reaction has yet to be reported. Here, we introduce a superaerophobic nitrogen-doped tungsten carbide nanoarray electrode exhibiting high stability and activity toward hydrogen evolution reaction as well as driving oxygen evolution efficiently in acid. Nitrogen-doping and nanoarray structure accelerate hydrogen gas release from the electrode, realizing a current density of -200 mA cm-2 at the potential of -190 mV vs. reversible hydrogen electrode, which manifest one of the best non-noble metal catalysts for hydrogen evolution reaction. Under acidic conditions (0.5 M sulfuric acid), water splitting catalyzed by nitrogen-doped tungsten carbide nanoarray starts from about 1.4 V, and outperforms most other water splitting catalysts.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [3];  [1]
  1. Beijing Univ. of Chemical Technology (China). State Key Lab. of Chemical Resource Engineering
  2. Yale Univ., New Haven, CT (United States). Dept. of Chemistry and Energy Sciences Inst.
  3. Beijing Univ. of Chemical Technology (China). State Key Lab. of Chemical Resource Engineering; Yale Univ., New Haven, CT (United States). Dept. of Chemistry and Energy Sciences Inst.
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1490192
Grant/Contract Number:  
SC0001059
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; 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

Han, Nana, Yang, Ke R., Lu, Zhiyi, Li, Yingjie, Xu, Wenwen, Gao, Tengfei, Cai, Zhao, Zhang, Ying, Batista, Victor S., Liu, Wen, and Sun, Xiaoming. Nitrogen-doped tungsten carbide nanoarray as an efficient bifunctional electrocatalyst for water splitting in acid. United States: N. p., 2018. Web. doi:10.1038/s41467-018-03429-z.
Han, Nana, Yang, Ke R., Lu, Zhiyi, Li, Yingjie, Xu, Wenwen, Gao, Tengfei, Cai, Zhao, Zhang, Ying, Batista, Victor S., Liu, Wen, & Sun, Xiaoming. Nitrogen-doped tungsten carbide nanoarray as an efficient bifunctional electrocatalyst for water splitting in acid. United States. https://doi.org/10.1038/s41467-018-03429-z
Han, Nana, Yang, Ke R., Lu, Zhiyi, Li, Yingjie, Xu, Wenwen, Gao, Tengfei, Cai, Zhao, Zhang, Ying, Batista, Victor S., Liu, Wen, and Sun, Xiaoming. Fri . "Nitrogen-doped tungsten carbide nanoarray as an efficient bifunctional electrocatalyst for water splitting in acid". United States. https://doi.org/10.1038/s41467-018-03429-z. https://www.osti.gov/servlets/purl/1490192.
@article{osti_1490192,
title = {Nitrogen-doped tungsten carbide nanoarray as an efficient bifunctional electrocatalyst for water splitting in acid},
author = {Han, Nana and Yang, Ke R. and Lu, Zhiyi and Li, Yingjie and Xu, Wenwen and Gao, Tengfei and Cai, Zhao and Zhang, Ying and Batista, Victor S. and Liu, Wen and Sun, Xiaoming},
abstractNote = {Tungsten carbide is one of the most promising electrocatalysts for the hydrogen evolution reaction, although it exhibits sluggish kinetics due to a strong tungsten-hydrogen bond. In addition, tungsten carbide’s catalytic activity toward the oxygen evolution reaction has yet to be reported. Here, we introduce a superaerophobic nitrogen-doped tungsten carbide nanoarray electrode exhibiting high stability and activity toward hydrogen evolution reaction as well as driving oxygen evolution efficiently in acid. Nitrogen-doping and nanoarray structure accelerate hydrogen gas release from the electrode, realizing a current density of -200 mA cm-2 at the potential of -190 mV vs. reversible hydrogen electrode, which manifest one of the best non-noble metal catalysts for hydrogen evolution reaction. Under acidic conditions (0.5 M sulfuric acid), water splitting catalyzed by nitrogen-doped tungsten carbide nanoarray starts from about 1.4 V, and outperforms most other water splitting catalysts.},
doi = {10.1038/s41467-018-03429-z},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Fri Mar 02 00:00:00 EST 2018},
month = {Fri Mar 02 00:00:00 EST 2018}
}

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Figures / Tables:

Fig. 1 Fig. 1: DFT hydrogen binding geometries and binding energies. Hydrogen binding geometries and binding energies of a WC (001) surface, b N-WC (001) surface, c Pt (111) surface, and d calculated partial density of state (DOS) of WC (001) and N-WC (001). The vertical dash line denotes the position ofmore » the Fermi level. Color key: black, brown, white, blue, and gray balls represent C, W, H, N, and Pt atoms, respectively« less

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Boosting hydrogen evolution activity of vanadyl pyrophosphate nanosheets for electrocatalytic overall water splitting
journal, January 2019

  • Zhang, Chaoxiong; Liu, Haoxuan; He, Jia
  • Chemical Communications, Vol. 55, Issue 71
  • DOI: 10.1039/c9cc04481g

Facile synthesis of amorphous MoS x –Fe anchored on Zr-MOFs towards efficient and stable electrocatalytic hydrogen evolution
journal, January 2020

  • Zhang, Le; Yan, Zhenhua; Chen, Xiang
  • Chemical Communications, Vol. 56, Issue 18
  • DOI: 10.1039/c9cc08771k

Mass-producible 2D-WS 2 bulk modified screen printed electrodes towards the hydrogen evolution reaction
journal, January 2019

  • Hughes, Jack P.; Blanco, Felipe D.; Banks, Craig E.
  • RSC Advances, Vol. 9, Issue 43
  • DOI: 10.1039/c9ra05342e

Constructing ultrathin CoP nanomeshes by Er-doping for highly efficient bifunctional electrocatalysts for overall water splitting
journal, January 2019

  • Zhang, Gengwei; Wang, Bin; Bi, Jinglei
  • Journal of Materials Chemistry A, Vol. 7, Issue 10
  • DOI: 10.1039/c9ta00530g

Interfacial nickel nitride/sulfide as a bifunctional electrode for highly efficient overall water/seawater electrolysis
journal, January 2019

  • Zhao, Yongqiang; Jin, Bo; Vasileff, Anthony
  • Journal of Materials Chemistry A, Vol. 7, Issue 14
  • DOI: 10.1039/c9ta01903k

Microwave-assisted ultrafast synthesis of adjustable bimetal phosphide/graphene heterostructures from MOFs for efficient electrochemical water splitting
journal, January 2019

  • Bu, Fanxing; Chen, Wenshu; Aly Aboud, Mohamed F.
  • Journal of Materials Chemistry A, Vol. 7, Issue 24
  • DOI: 10.1039/c9ta03146d

A universal synthesis strategy to make metal nitride electrocatalysts for hydrogen evolution reaction
journal, January 2019

  • Yu, Luo; Song, Shaowei; McElhenny, Brian
  • Journal of Materials Chemistry A, Vol. 7, Issue 34
  • DOI: 10.1039/c9ta05455c

Tailoring the facets of Ni 3 S 2 as a bifunctional electrocatalyst for high-performance overall water-splitting
journal, January 2019

  • Li, Lingjie; Sun, Caiyun; Shang, Bo
  • Journal of Materials Chemistry A, Vol. 7, Issue 30
  • DOI: 10.1039/c9ta05578a

Activating and optimizing the activity of NiCoP nanosheets for electrocatalytic alkaline water splitting through the V doping effect enhanced by P vacancies
journal, January 2019

  • Yan, Yaotian; Lin, Jinghuang; Cao, Jian
  • Journal of Materials Chemistry A, Vol. 7, Issue 42
  • DOI: 10.1039/c9ta09283h

Facile Synthesis of Tungsten Carbide Nanosheets for Trace Level Detection of Toxic Mercury Ions in Biological and Contaminated Sewage Water Samples: An Electrocatalytic Approach
journal, January 2019

  • Boopathy, Gopal; Govindasamy, Mani; Nazari, Maryam
  • Journal of The Electrochemical Society, Vol. 166, Issue 10
  • DOI: 10.1149/2.0181910jes

Earth-Abundant Electrocatalysts in Proton Exchange Membrane Electrolyzers
journal, December 2018

  • Sun, Xinwei; Xu, Kaiqi; Fleischer, Christian
  • Catalysts, Vol. 8, Issue 12
  • DOI: 10.3390/catal8120657

Self‐Supported Transition‐Metal‐Based Electrocatalysts for Hydrogen and Oxygen Evolution
journal, April 2019


Surface‐Electron Coupling for Efficient Hydrogen Evolution
journal, December 2019

  • Fu, Weiwei; Wang, Yanwei; Hu, Jisong
  • Angewandte Chemie International Edition, Vol. 58, Issue 49
  • DOI: 10.1002/anie.201908938

Constructing Earth‐abundant 3D Nanoarrays for Efficient Overall Water Splitting – A Review
journal, February 2019

  • Jamesh, Mohammed‐Ibrahim; Kuang, Yun; Sun, Xiaoming
  • ChemCatChem, Vol. 11, Issue 6
  • DOI: 10.1002/cctc.201801783

Morphology and surface chemistry engineering toward pH-universal catalysts for hydrogen evolution at high current density
journal, January 2019


A Ni-loaded, metal–organic framework–graphene composite as a precursor for in situ electrochemical deposition of a highly active and durable water oxidation nanocatalyst
journal, January 2019

  • Hassan, Mohamed H.; Soliman, Ahmed B.; Elmehelmey, Worood A.
  • Chemical Communications, Vol. 55, Issue 1
  • DOI: 10.1039/c8cc07120a

Oxygen vacancy-assisted hydrogen evolution reaction of the Pt/WO 3 electrocatalyst
journal, January 2019

  • Tian, Han; Cui, Xiangzhi; Zeng, Liming
  • Journal of Materials Chemistry A, Vol. 7, Issue 11
  • DOI: 10.1039/c8ta12219a

Cu 3 N nanowire array as a high-efficiency and durable electrocatalyst for oxygen evolution reaction
journal, January 2019

  • Guo, Huanmei; Liu, Li; Wu, Qian
  • Dalton Transactions, Vol. 48, Issue 16
  • DOI: 10.1039/c9dt00362b

Edge-oriented MoS 2 supported on nickel/carbon core–shell nanospheres for enhanced hydrogen evolution reaction performance
journal, January 2019

  • Wang, Yin; Wang, Zegao; Yang, Qian
  • New Journal of Chemistry, Vol. 43, Issue 16
  • DOI: 10.1039/c9nj00612e

Cation-tunable flower-like (Ni x Fe 1−x ) 2 P@graphitized carbon films as ultra-stable electrocatalysts for overall water splitting in alkaline media
journal, January 2019

  • Zhao, Hongyang; Wang, Yanwei; Fang, Ling
  • Journal of Materials Chemistry A, Vol. 7, Issue 35
  • DOI: 10.1039/c9ta07762f

Epitaxial Heterogeneous Interfaces on N-NiMoO 4 /NiS 2 Nanowires/Nanosheets to Boost Hydrogen and Oxygen Production for Overall Water Splitting
journal, November 2018

  • An, Li; Feng, Jianrui; Zhang, Yu
  • Advanced Functional Materials, Vol. 29, Issue 1
  • DOI: 10.1002/adfm.201805298

In situ construction of graphdiyne/CuS heterostructures for efficient hydrogen evolution reaction
journal, January 2019

  • Shi, Guodong; Fan, Zixiong; Du, Lili
  • Materials Chemistry Frontiers, Vol. 3, Issue 5
  • DOI: 10.1039/c9qm00064j

Morphology and surface chemistry engineering toward pH-universal catalysts for hydrogen evolution at high current density
journal, January 2019


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.