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

Han, Nana; Yang, Ke R.; Lu, Zhiyi; Li, Yingjie; Xu, Wenwen; Gao, Tengfei; Cai, Zhao; Zhang, Ying; Batista, Victor S.; Liu, Wen; Sun, Xiaoming

doi:10.1038/s41467-018-03429-z

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

Journal Article · 02 March 2018 · Nature Communications

DOI: https://doi.org/10.1038/s41467-018-03429-z · OSTI ID:1490192

Han, Nana ^[1]; Yang, Ke R. ^[2]; Lu, Zhiyi ^[1]; Li, Yingjie ^[1]; Xu, Wenwen ^[1]; Gao, Tengfei ^[1]; Cai, Zhao ^[1]; Zhang, Ying ^[1]; Batista, Victor S. ^[2];

^[3]; Sun, Xiaoming ^[1]

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.
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.

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.

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Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001059

OSTI ID:: 1490192

Journal Information:: Nature Communications, Vol. 9, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 533 works

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Molecular Insight in Structure and Activity of Highly Efficient, Low-Ir Ir–Ni Oxide Catalysts for Electrochemical Water Splitting (OER) Reier, Tobias; Pawolek, Zarina; Cherevko, Serhiy Journal of the American Chemical Society, Vol. 137, Issue 40 https://doi.org/10.1021/jacs.5b07788	journal	September 2015
Cage-Confinement Pyrolysis Route to Ultrasmall Tungsten Carbide Nanoparticles for Efficient Electrocatalytic Hydrogen Evolution Xu, Yan-Tong; Xiao, Xiaofen; Ye, Zi-Ming Journal of the American Chemical Society, Vol. 139, Issue 15 https://doi.org/10.1021/jacs.7b00165	journal	April 2017
A Comparison of the Adsorption and Diffusion of Hydrogen on the {111} Surfaces of Ni, Pd, and Pt from Density Functional Theory Calculations Watson, Graeme W.; Wells, Richard P. K.; Willock, David J. The Journal of Physical Chemistry B, Vol. 105, Issue 21 https://doi.org/10.1021/jp002864c	journal	May 2001
Hydrogen-storage materials for mobile applications Schlapbach, Louis; Züttel, Andreas Nature, Vol. 414, Issue 6861 https://doi.org/10.1038/35104634	journal	November 2001
Hybrid bio-photo-electro-chemical cells for solar water splitting Pinhassi, Roy I.; Kallmann, Dan; Saper, Gadiel Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12552	journal	August 2016
Ultrasmall and phase-pure W2C nanoparticles for efficient electrocatalytic and photoelectrochemical hydrogen evolution Gong, Qiufang; Wang, Yu; Hu, Qi Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13216	journal	October 2016
Hydrogen evolution from a copper(I) oxide photocathode coated with an amorphous molybdenum sulphide catalyst Morales-Guio, Carlos G.; Tilley, S. David; Vrubel, Heron Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4059	journal	January 2014
Modification of the surface electronic and chemical properties of Pt(111) by subsurface 3d transition metals Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A. The Journal of Chemical Physics, Vol. 120, Issue 21 https://doi.org/10.1063/1.1737365	journal	June 2004
Sustainable Hydrogen Production Turner, J. A. Science, Vol. 305, Issue 5686 https://doi.org/10.1126/science.1103197	journal	August 2004
Platinum-Like Behavior of Tungsten Carbide in Surface Catalysis Levy, R. B.; Boudart, M. Science, Vol. 181, Issue 4099 https://doi.org/10.1126/science.181.4099.547	journal	August 1973
Surface Electronic Properties of Tungsten, Tungsten Carbide, and Platinum Houston, J. E.; Laramore, G. E.; Park, R. L. Science, Vol. 185, Issue 4147 https://doi.org/10.1126/science.185.4147.258	journal	July 1974
Theoretical analysis of doped graphene as cathode catalyst in Li-O2 and Na-O2 batteries -- the impact of the computational scheme Novčić, Katarina A.; Dobrota, Ana S.; Petković, Milena arXiv https://doi.org/10.48550/arxiv.2006.12912	preprint	January 2020

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Co and Fe Codoped WO 2.72 as Alkaline‐Solution‐Available Oxygen Evolution Reaction Catalyst to Construct Photovoltaic Water Splitting System with Solar‐To‐Hydrogen Efficiency of 16.9% Chen, Huayu; Song, Lizhu; Ouyang, Shuxin Advanced Science, Vol. 6, Issue 16 https://doi.org/10.1002/advs.201900465	journal	June 2019
Construction of Hierarchical Co–Fe Oxyphosphide Microtubes for Electrocatalytic Overall Water Splitting Zhang, Peng; Lu, Xue Feng; Nai, Jianwei Advanced Science, Vol. 6, Issue 17 https://doi.org/10.1002/advs.201900576	journal	July 2019
Rational Design of Holey 2D Nonlayered Transition Metal Carbide/Nitride Heterostructure Nanosheets for Highly Efficient Water Oxidation Kou, Zongkui; Wang, Tingting; Gu, Qilin Advanced Energy Materials, Vol. 9, Issue 16 https://doi.org/10.1002/aenm.201803768	journal	February 2019
Synergistically Tuning Water and Hydrogen Binding Abilities Over Co 4 N by Cr Doping for Exceptional Alkaline Hydrogen Evolution Electrocatalysis Yao, Na; Li, Peng; Zhou, Zirui Advanced Energy Materials, Vol. 9, Issue 41 https://doi.org/10.1002/aenm.201902449	journal	September 2019
Atomically Dispersed Mo Supported on Metallic Co ₉ S ₈ Nanoflakes as an Advanced Noble‐Metal‐Free Bifunctional Water Splitting Catalyst Working in Universal pH Conditions Wang, Ligang; Duan, Xinxuan; Liu, Xijun Advanced Energy Materials, Vol. 10, Issue 4 https://doi.org/10.1002/aenm.201903137	journal	December 2019
Organic Proton‐Buffer Electrode to Separate Hydrogen and Oxygen Evolution in Acid Water Electrolysis Ma, Yuanyuan; Guo, Zhaowei; Dong, Xiaoli Angewandte Chemie, Vol. 131, Issue 14 https://doi.org/10.1002/ange.201814625	journal	February 2019
Interfacial Defect Engineering for Improved Portable Zinc–Air Batteries with a Broad Working Temperature An, Li; Huang, Bolong; Zhang, Yu Angewandte Chemie, Vol. 131, Issue 28 https://doi.org/10.1002/ange.201903879	journal	June 2019
Promoting Subordinate, Efficient Ruthenium Sites with Interstitial Silicon for Pt‐Like Electrocatalytic Activity Chen, Hui; Ai, Xuan; Liu, Wang Angewandte Chemie https://doi.org/10.1002/ange.201906394	journal	July 2019
Surface‐Electron Coupling for Efficient Hydrogen Evolution Fu, Weiwei; Wang, Yanwei; Hu, Jisong Angewandte Chemie, Vol. 131, Issue 49 https://doi.org/10.1002/ange.201908938	journal	October 2019
Organic Proton‐Buffer Electrode to Separate Hydrogen and Oxygen Evolution in Acid Water Electrolysis Ma, Yuanyuan; Guo, Zhaowei; Dong, Xiaoli Angewandte Chemie International Edition, Vol. 58, Issue 14 https://doi.org/10.1002/anie.201814625	journal	February 2019
Promoting Subordinate, Efficient Ruthenium Sites with Interstitial Silicon for Pt-Like Electrocatalytic Activity Chen, Hui; Ai, Xuan; Liu, Wang Angewandte Chemie International Edition, Vol. 58, Issue 33 https://doi.org/10.1002/anie.201906394	journal	July 2019
Nanotubes of NiCo ₂ S ₄ /Co ₉ S ₈ Heterostructure: Efficient Hydrogen Evolution Catalyst in Alkaline Medium Basu, Mrinmoyee Chemistry - An Asian Journal, Vol. 13, Issue 21 https://doi.org/10.1002/asia.201801185	journal	October 2018
Noble‐Metal‐Free Colloidal‐Copper Based Low Overpotential Water Oxidation Electrocatalyst Babar, Noor‐Ul‐Ain; Joya, Khurram Saleem; Ehsan, Muhammad Ali ChemCatChem, Vol. 11, Issue 24 https://doi.org/10.1002/cctc.201900202	journal	July 2019
Modulating Schottky Barrier of MoS ₂ to Enhance Hydrogen Evolution Reaction Activity by Incorporating with Vertical Graphene Nanosheets Derived from Organic Liquid Waste Wu, Angjian; Xu, Aoni; Yang, Jian ChemElectroChem, Vol. 5, Issue 24 https://doi.org/10.1002/celc.201801279	journal	November 2018
Cobalt‐Embedded N‐Doped Carbon Arrays Derived In Situ as Trifunctional Catalyst Toward Hydrogen and Oxygen Evolution, and Oxygen Reduction Huang, Niu; Yang, Liu; Zhang, Mingyi ChemElectroChem, Vol. 6, Issue 17 https://doi.org/10.1002/celc.201901106	journal	August 2019
Nonmetal Doping as a Robust Route for Boosting the Hydrogen Evolution of Metal‐Based Electrocatalysts Hu, Qi; Li, Guomin; Han, Zhen Chemistry – A European Journal https://doi.org/10.1002/chem.201902998	journal	August 2019
Solid‐State Conversion Synthesis of Advanced Electrocatalysts for Water Splitting Ma, Xiaomin; Shi, Yanmei; Wang, Kang Chemistry – A European Journal https://doi.org/10.1002/chem.201904021	journal	December 2019
WX _y /g‐C ₃ N ₄ (WX _y =W ₂ C, WS ₂ , or W ₂ N) Composites for Highly Efficient Photocatalytic Water Splitting Shao, Mengmeng; Chen, Wenzhou; Ding, Shengjie ChemSusChem, Vol. 12, Issue 14 https://doi.org/10.1002/cssc.201900844	journal	June 2019
Self‐Assembled Monolayer Stabilized Gold‐Vanadate Nanoflute for Water Splitting Reactions Das, Biraj; Sharma, Mukesh; Hazarika, Anil ChemistrySelect, Vol. 4, Issue 24 https://doi.org/10.1002/slct.201901715	journal	June 2019
Twinned Tungsten Carbonitride Nanocrystals Boost Hydrogen Evolution Activity and Stability Kou, Zongkui; Wang, Tingting; Wu, Haijun Small, Vol. 15, Issue 19 https://doi.org/10.1002/smll.201900248	journal	April 2019
Fibrous‐Structured Freestanding Electrodes for Oxygen Electrocatalysis Jiang, Shan; Li, Jingliang; Fang, Jian Small https://doi.org/10.1002/smll.201903760	journal	December 2019
Phosphorus and Yttrium Codoped Co(OH)F Nanoarray as Highly Efficient and Bifunctional Electrocatalysts for Overall Water Splitting Zhang, Gengwei; Wang, Bin; Li, Lu Small, Vol. 15, Issue 42 https://doi.org/10.1002/smll.201904105	journal	August 2019
Amorphous Catalysts and Electrochemical Water Splitting: An Untold Story of Harmony Anantharaj, Sengeni; Noda, Suguru Small, Vol. 16, Issue 2 https://doi.org/10.1002/smll.201905779	journal	December 2019
WC _1−x ‐Coupled 3D Porous Defective g‐C ₃ N ₄ for Efficient Photocatalytic Overall Water Splitting Xiong, Ye; Chen, Yipeng; Yang, Ning Solar RRL, Vol. 3, Issue 5 https://doi.org/10.1002/solr.201800341	journal	February 2019
Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide Xia, Chuan; Back, Seoin; Ringe, Stefan Nature Catalysis, Vol. 3, Issue 2 https://doi.org/10.1038/s41929-019-0402-8	journal	January 2020
VS ₂ : an efficient catalyst for an electrochemical hydrogen evolution reaction in an acidic medium Das, Jiban K.; Samantara, Aneeya K.; Nayak, Arpan K. Dalton Transactions, Vol. 47, Issue 39 https://doi.org/10.1039/c8dt02547a	journal	January 2018
Ultrafast fabrication of nickel sulfide film on Ni foam for efficient overall water splitting Ren, Gang; Hao, Qiuyan; Mao, Jing Nanoscale, Vol. 10, Issue 36 https://doi.org/10.1039/c8nr05494k	journal	January 2018
Activation of defective nickel molybdate nanowires for enhanced alkaline electrochemical hydrogen evolution An, Li; Zhang, Yu; Wang, Rui Nanoscale, Vol. 10, Issue 35 https://doi.org/10.1039/c8nr05723k	journal	January 2018
W ₂ C nanodot-decorated CNT networks as a highly efficient and stable electrocatalyst for hydrogen evolution in acidic and alkaline media Hu, Yang; Yu, Bo; Li, Wenxin Nanoscale, Vol. 11, Issue 11 https://doi.org/10.1039/c8nr10281c	journal	January 2019
Well-aligned metal–organic framework array-derived CoS ₂ nanosheets toward robust electrochemical water splitting Yao, Na; Tan, Tan; Yang, Fulin Materials Chemistry Frontiers, Vol. 2, Issue 9 https://doi.org/10.1039/c8qm00259b	journal	January 2018
Defect-rich (Co–CoS ₂ ) _x @Co ₉ S ₈ nanosheets derived from monomolecular precursor pyrolysis with excellent catalytic activity for hydrogen evolution reaction Zhang, Xinwen; Liu, Yanyan; Gao, Jie Journal of Materials Chemistry A, Vol. 6, Issue 17 https://doi.org/10.1039/c8ta01163j	journal	January 2018
Ultrafine cable-like WC/W ₂ C heterojunction nanowires covered by graphitic carbon towards highly efficient electrocatalytic hydrogen evolution Zhang, Lu-Nan; Ma, Yuan-Yuan; Lang, Zhong-Ling Journal of Materials Chemistry A, Vol. 6, Issue 31 https://doi.org/10.1039/c8ta05007d	journal	January 2018
Boosting hydrogen evolution activity of vanadyl pyrophosphate nanosheets for electrocatalytic overall water splitting Zhang, Chaoxiong; Liu, Haoxuan; He, Jia Chemical Communications, Vol. 55, Issue 71 https://doi.org/10.1039/c9cc04481g	journal	January 2019
Facile synthesis of amorphous MoS _x –Fe anchored on Zr-MOFs towards efficient and stable electrocatalytic hydrogen evolution Zhang, Le; Yan, Zhenhua; Chen, Xiang Chemical Communications, Vol. 56, Issue 18 https://doi.org/10.1039/c9cc08771k	journal	January 2020
Co,N-Codoped porous vanadium nitride nanoplates as superior bifunctional electrocatalysts for hydrogen evolution and oxygen reduction reactions Zhang, Ning; Cao, Liyun; Feng, Liangliang Nanoscale, Vol. 11, Issue 24 https://doi.org/10.1039/c9nr02637a	journal	January 2019
Mass-producible 2D-WS ₂ bulk modified screen printed electrodes towards the hydrogen evolution reaction Hughes, Jack P.; Blanco, Felipe D.; Banks, Craig E. RSC Advances, Vol. 9, Issue 43 https://doi.org/10.1039/c9ra05342e	journal	January 2019
Constructing ultrathin CoP nanomeshes by Er-doping for highly efficient bifunctional electrocatalysts for overall water splitting Zhang, Gengwei; Wang, Bin; Bi, Jinglei Journal of Materials Chemistry A, Vol. 7, Issue 10 https://doi.org/10.1039/c9ta00530g	journal	January 2019
Interfacial nickel nitride/sulfide as a bifunctional electrode for highly efficient overall water/seawater electrolysis Zhao, Yongqiang; Jin, Bo; Vasileff, Anthony Journal of Materials Chemistry A, Vol. 7, Issue 14 https://doi.org/10.1039/c9ta01903k	journal	January 2019
Microwave-assisted ultrafast synthesis of adjustable bimetal phosphide/graphene heterostructures from MOFs for efficient electrochemical water splitting Bu, Fanxing; Chen, Wenshu; Aly Aboud, Mohamed F. Journal of Materials Chemistry A, Vol. 7, Issue 24 https://doi.org/10.1039/c9ta03146d	journal	January 2019
A universal synthesis strategy to make metal nitride electrocatalysts for hydrogen evolution reaction Yu, Luo; Song, Shaowei; McElhenny, Brian Journal of Materials Chemistry A, Vol. 7, Issue 34 https://doi.org/10.1039/c9ta05455c	journal	January 2019
Activating and optimizing the activity of NiCoP nanosheets for electrocatalytic alkaline water splitting through the V doping effect enhanced by P vacancies Yan, Yaotian; Lin, Jinghuang; Cao, Jian Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/c9ta09283h	journal	January 2019
Facile Synthesis of Tungsten Carbide Nanosheets for Trace Level Detection of Toxic Mercury Ions in Biological and Contaminated Sewage Water Samples: An Electrocatalytic Approach Boopathy, Gopal; Govindasamy, Mani; Nazari, Maryam Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0181910jes	journal	January 2019
Earth-Abundant Electrocatalysts in Proton Exchange Membrane Electrolyzers Sun, Xinwei; Xu, Kaiqi; Fleischer, Christian Catalysts, Vol. 8, Issue 12 https://doi.org/10.3390/catal8120657	journal	December 2018
Polyoxometalate‐Derived Hexagonal Molybdenum Nitrides (MXenes) Supported by Boron, Nitrogen Codoped Carbon Nanotubes for Efficient Electrochemical Hydrogen Evolution from Seawater Miao, Jun; Lang, Zhongling; Zhang, Xinyu Advanced Functional Materials https://doi.org/10.1002/adfm.201805893	journal	December 2018
Self‐Supported Transition‐Metal‐Based Electrocatalysts for Hydrogen and Oxygen Evolution Sun, Hongming; Yan, Zhenhua; Liu, Fangming Advanced Materials, Vol. 32, Issue 3 https://doi.org/10.1002/adma.201806326	journal	April 2019
Surface‐Electron Coupling for Efficient Hydrogen Evolution Fu, Weiwei; Wang, Yanwei; Hu, Jisong Angewandte Chemie International Edition, Vol. 58, Issue 49 https://doi.org/10.1002/anie.201908938	journal	December 2019
Constructing Earth‐abundant 3D Nanoarrays for Efficient Overall Water Splitting – A Review Jamesh, Mohammed‐Ibrahim; Kuang, Yun; Sun, Xiaoming ChemCatChem, Vol. 11, Issue 6 https://doi.org/10.1002/cctc.201801783	journal	February 2019
Morphology and surface chemistry engineering toward pH-universal catalysts for hydrogen evolution at high current density Luo, Yuting; Tang, Lei; Khan, Usman Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-07792-9	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 Hassan, Mohamed H.; Soliman, Ahmed B.; Elmehelmey, Worood A. Chemical Communications, Vol. 55, Issue 1 https://doi.org/10.1039/c8cc07120a	journal	January 2019
Ultrafine CoPS nanoparticles encapsulated in N, P, and S tri-doped porous carbon as an efficient bifunctional water splitting electrocatalyst in both acid and alkaline solutions Hu, Yiping; Li, Feng; Long, Yu Journal of Materials Chemistry A, Vol. 6, Issue 22 https://doi.org/10.1039/c8ta01310a	journal	January 2018
Oxygen vacancy-assisted hydrogen evolution reaction of the Pt/WO ₃ electrocatalyst Tian, Han; Cui, Xiangzhi; Zeng, Liming Journal of Materials Chemistry A, Vol. 7, Issue 11 https://doi.org/10.1039/c8ta12219a	journal	January 2019
Fe/P dual doping boosts the activity and durability of CoS ₂ polycrystalline nanowires for hydrogen evolution Zhang, Yang-Yang; Zhang, Xing; Wu, Ze-Yuan Journal of Materials Chemistry A, Vol. 7, Issue 10 https://doi.org/10.1039/c8ta12269e	journal	January 2019
A robust electrocatalytic activity toward the hydrogen evolution reaction from W/W ₂ C heterostructured nanoparticles coated with a N,P dual-doped carbon layer Zhang, Quan; Luo, Fang; Hu, Hao Chemical Communications, Vol. 55, Issue 65 https://doi.org/10.1039/c9cc04318g	journal	January 2019
Cu ₃ N nanowire array as a high-efficiency and durable electrocatalyst for oxygen evolution reaction Guo, Huanmei; Liu, Li; Wu, Qian Dalton Transactions, Vol. 48, Issue 16 https://doi.org/10.1039/c9dt00362b	journal	January 2019
Edge-oriented MoS ₂ supported on nickel/carbon core–shell nanospheres for enhanced hydrogen evolution reaction performance Wang, Yin; Wang, Zegao; Yang, Qian New Journal of Chemistry, Vol. 43, Issue 16 https://doi.org/10.1039/c9nj00612e	journal	January 2019
Epitaxial Heterogeneous Interfaces on N-NiMoO ₄ /NiS ₂ Nanowires/Nanosheets to Boost Hydrogen and Oxygen Production for Overall Water Splitting An, Li; Feng, Jianrui; Zhang, Yu Advanced Functional Materials, Vol. 29, Issue 1 https://doi.org/10.1002/adfm.201805298	journal	November 2018
In situ construction of graphdiyne/CuS heterostructures for efficient hydrogen evolution reaction Shi, Guodong; Fan, Zixiong; Du, Lili Materials Chemistry Frontiers, Vol. 3, Issue 5 https://doi.org/10.1039/c9qm00064j	journal	January 2019
Morphology and surface chemistry engineering toward pH-universal catalysts for hydrogen evolution at high current density Luo, Yuting; Tang, Lei; Khan, Usman Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-07792-9	journal	January 2019