Atomically Engineering Activation Sites Onto Metallic 1T-MoS Catalysts for Enhanced Electrochemical Hydrogen Evolution

Overview

Journal Nat Commun

Specialty Biology

Date 2019 Mar 1

PMID 30816110

Citations 35

Authors

Yichao Huang

Yuanhui Sun

Xueli Zheng

Toshihiro Aoki

Brian Pattengale

Jier Huang

Xin He

Wei Bian

Sabrina Younan

Nicholas Williams

Jun Hu

Jingxuan Ge

Ning Pu

Xingxu Yan

Xiaoqing Pan

Lijun Zhang

Yongge Wei

Jing Gu

Affiliations

Soon will be listed here.

Abstract

Engineering catalytic sites at the atomic level provides an opportunity to understand the catalyst's active sites, which is vital to the development of improved catalysts. Here we show a reliable and tunable polyoxometalate template-based synthetic strategy to atomically engineer metal doping sites onto metallic 1T-MoS, using Anderson-type polyoxometalates as precursors. Benefiting from engineering nickel and oxygen atoms, the optimized electrocatalyst shows great enhancement in the hydrogen evolution reaction with a positive onset potential of ~ 0 V and a low overpotential of -46 mV in alkaline electrolyte, comparable to platinum-based catalysts. First-principles calculations reveal co-doping nickel and oxygen into 1T-MoS assists the process of water dissociation and hydrogen generation from their intermediate states. This research will expand on the ability to improve the activities of various catalysts by precisely engineering atomic activation sites to achieve significant electronic modulations and improve atomic utilization efficiencies.

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References

Greeley J, Jaramillo T, Bonde J, Chorkendorff I, Norskov J . Computational high-throughput screening of electrocatalytic materials for hydrogen evolution. Nat Mater. 2006; 5(11):909-13. DOI: 10.1038/nmat1752. View

Jin Y, Wang H, Li J, Yue X, Han Y, Shen P . Porous MoO2 Nanosheets as Non-noble Bifunctional Electrocatalysts for Overall Water Splitting. Adv Mater. 2016; 28(19):3785-90. DOI: 10.1002/adma.201506314. View

Eda G, Fujita T, Yamaguchi H, Voiry D, Chen M, Chhowalla M . Coherent atomic and electronic heterostructures of single-layer MoS2. ACS Nano. 2012; 6(8):7311-7. DOI: 10.1021/nn302422x. View

Geng X, Sun W, Wu W, Chen B, Al-Hilo A, Benamara M . Pure and stable metallic phase molybdenum disulfide nanosheets for hydrogen evolution reaction. Nat Commun. 2016; 7:10672. PMC: 4749985. DOI: 10.1038/ncomms10672. View

Xu Y, Kraft M, Xu R . Metal-free carbonaceous electrocatalysts and photocatalysts for water splitting. Chem Soc Rev. 2016; 45(11):3039-52. DOI: 10.1039/c5cs00729a. View

Yin Q, Tan J, Besson C, Geletii Y, Musaev D, Kuznetsov A . A fast soluble carbon-free molecular water oxidation catalyst based on abundant metals. Science. 2010; 328(5976):342-5. DOI: 10.1126/science.1185372. View

Kibsgaard J, Chen Z, Reinecke B, Jaramillo T . Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis. Nat Mater. 2012; 11(11):963-9. DOI: 10.1038/nmat3439. View

Li H, Du M, Mleczko M, Koh A, Nishi Y, Pop E . Kinetic Study of Hydrogen Evolution Reaction over Strained MoS2 with Sulfur Vacancies Using Scanning Electrochemical Microscopy. J Am Chem Soc. 2016; 138(15):5123-9. DOI: 10.1021/jacs.6b01377. View

Zhu Y, Guo C, Zheng Y, Qiao S . Surface and Interface Engineering of Noble-Metal-Free Electrocatalysts for Efficient Energy Conversion Processes. Acc Chem Res. 2017; 50(4):915-923. DOI: 10.1021/acs.accounts.6b00635. View

10.

Yan H, Tian C, Wang L, Wu A, Meng M, Zhao L . Phosphorus-modified tungsten nitride/reduced graphene oxide as a high-performance, non-noble-metal electrocatalyst for the hydrogen evolution reaction. Angew Chem Int Ed Engl. 2015; 54(21):6325-9. DOI: 10.1002/anie.201501419. View

11.

Tsai C, Li H, Park S, Park J, Han H, Norskov J . Electrochemical generation of sulfur vacancies in the basal plane of MoS for hydrogen evolution. Nat Commun. 2017; 8():15113. PMC: 5530599. DOI: 10.1038/ncomms15113. View

12.

Wang P, Zhang X, Zhang J, Wan S, Guo S, Lu G . Precise tuning in platinum-nickel/nickel sulfide interface nanowires for synergistic hydrogen evolution catalysis. Nat Commun. 2017; 8:14580. PMC: 5333357. DOI: 10.1038/ncomms14580. View

13.

Lv H, Geletii Y, Zhao C, Vickers J, Zhu G, Luo Z . Polyoxometalate water oxidation catalysts and the production of green fuel. Chem Soc Rev. 2012; 41(22):7572-89. DOI: 10.1039/c2cs35292c. View

14.

Xie J, Zhang J, Li S, Grote F, Zhang X, Zhang H . Controllable disorder engineering in oxygen-incorporated MoS2 ultrathin nanosheets for efficient hydrogen evolution. J Am Chem Soc. 2013; 135(47):17881-8. DOI: 10.1021/ja408329q. View

15.

Sun Y, Hu X, Luo W, Huang Y . Self-assembled hierarchical MoO2/graphene nanoarchitectures and their application as a high-performance anode material for lithium-ion batteries. ACS Nano. 2011; 5(9):7100-7. DOI: 10.1021/nn201802c. View

16.

Voiry D, Fullon R, Yang J, de Carvalho Castro E Silva C, Kappera R, Bozkurt I . The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen. Nat Mater. 2016; 15(9):1003-9. DOI: 10.1038/nmat4660. View

17.

Wang H, Lee H, Deng Y, Lu Z, Hsu P, Liu Y . Bifunctional non-noble metal oxide nanoparticle electrocatalysts through lithium-induced conversion for overall water splitting. Nat Commun. 2015; 6:7261. PMC: 4557299. DOI: 10.1038/ncomms8261. View

18.

Li G, Zhang D, Qiao Q, Yu Y, Peterson D, Zafar A . All The Catalytic Active Sites of MoS for Hydrogen Evolution. J Am Chem Soc. 2016; 138(51):16632-16638. DOI: 10.1021/jacs.6b05940. View

19.

Hinnemann B, Moses P, Bonde J, Jorgensen K, Nielsen J, Horch S . Biomimetic hydrogen evolution: MoS2 nanoparticles as catalyst for hydrogen evolution. J Am Chem Soc. 2005; 127(15):5308-9. DOI: 10.1021/ja0504690. View

20.

Chhowalla M, Shin H, Eda G, Li L, Loh K, Zhang H . The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets. Nat Chem. 2013; 5(4):263-75. DOI: 10.1038/nchem.1589. View