All The Catalytic Active Sites of MoS 2 for Hydrogen Evolution
Open accessAbstract
MoS 2 presents a promising low-cost catalyst for the hydrogen evolution reaction (HER), but the understanding about its active sites has remained limited. Here we present an unambiguous study of the catalytic activities of all possible reaction sites of MoS 2, including edge sites, sulfur vacancies, and grain boundaries. We demonstrate that, in addition to the well-known catalytically active edge sites, sulfur vacancies provide another major active site for the HER, while the catalytic activity of grain boundaries is much weaker. The intrinsic turnover frequencies (Tafel slopes) of the edge sites, sulfur vacancies, and grain boundaries are estimated to be 7.5 s –1 (65–75 mV/dec), 3.2 s –1 (65–85 mV/dec), and 0.1 s –1 (120–160 mV/dec), respectively. We also demonstrate that the catalytic activity of sulfur vacancies strongly depends on the density of the vacancies and the local crystalline structure in proximity to the vacancies. Unlike edge sites, whose catalytic activity linearly depends on the length, sulfur vacancies show optimal catalytic activities when the vacancy density is in the range of 7–10%, and the number of sulfur vacancies in high crystalline quality MoS 2 is higher than that in low crystalline quality MoS 2, which may be related with the proximity of different local crystalline structures to the vacancies.
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Cites
Generalized Gradient Approximation Made Simple
Perdew, J. P., Burke, K., & Ernzerhof, M. (1996) · Physical Review Letters · doi:10.1103/physrevlett.77.3865 · Cited by 215,824 · see citing works
Kresse, G., & Furthmüller, J. (1996) · Physical Review B · doi:10.1103/physrevb.54.11169 · Cited by 123,652 · see citing works
Special points for Brillouin-zone integrations
Monkhorst, H. J., & Pack, J. D. (1976) · Physical Review B · doi:10.1103/physrevb.13.5188 · Cited by 71,721 · see citing works
Jaramillo, T. F., Jørgensen, K. P., Bonde, J., Nielsen, J. H., Horch, S., & Chorkendorff, I. (2007) · Science · doi:10.1126/science.1141483 · Cited by 6,100 · see citing works
Li, Y., Wang, H., Xie, L., Liang, Y., Hong, G., & Dai, H. (2011) · Journal of the American Chemical Society · doi:10.1021/ja201269b · Cited by 5,001 · see citing works
Biomimetic Hydrogen Evolution: MoS <sub>2</sub> Nanoparticles as Catalyst for Hydrogen Evolution
Hinnemann, B., Moses, P. G., Bonde, J., Jørgensen, K. P., Nielsen, J. H., Horch, S., Chorkendorff, I., & Nørskov, J. K. (2005) · Journal of the American Chemical Society · doi:10.1021/ja0504690 · Cited by 4,065 · see citing works
Synthesis of Large‐Area MoS<sub>2</sub> Atomic Layers with Chemical Vapor Deposition
Lee, Y., Zhang, X., Zhang, W., Chang, M., Lin, C., Chang, K., Yu, Y., Wang, J. T., Chang, C., Li, L., et al. (2012) · Advanced Materials · doi:10.1002/adma.201104798 · Cited by 3,422 · see citing works
Self-citationLukowski, M. A., Daniel, A. S., Meng, F., Forticaux, A., Li, L., & Jin, S. (2013) · Journal of the American Chemical Society · doi:10.1021/ja404523s · Cited by 3,341 · see citing works
Kibsgaard, J., Chen, Z., Reinecke, B. N., & Jaramillo, T. F. (2012) · Nature Materials · doi:10.1038/nmat3439 · Cited by 3,234 · see citing works
Enhanced catalytic activity in strained chemically exfoliated WS2 nanosheets for hydrogen evolution
Voiry, D., Yamaguchi, H., Li, J., Silva, R., Alves, D. C. B., Fujita, T., Chen, M., Asefa, T., Shenoy, V. B., Eda, G., et al. (2013) · Nature Materials · doi:10.1038/nmat3700 · Cited by 2,641 · see citing works
Li, H., Tsai, C., Koh, A. L., Cai, L., Contryman, A. W., Fragapane, A. H., Zhao, J., Han, H. S., Manoharan, H. C., Abild-Pedersen, F., et al. (2016) · Nature Materials · doi:10.1038/nmat4465 · Cited by 2,529 · see citing works
Xie, J., Zhang, J., Li, S., Grote, F., Zhang, X., Zhang, H., Wang, R., Lei, Y., Pan, B., & Xie, Y. (2013) · Journal of the American Chemical Society · doi:10.1021/ja408329q · Cited by 2,350 · see citing works
Synthesis of MoS <sub>2</sub> and MoSe <sub>2</sub> Films with Vertically Aligned Layers
Kong, D., Wang, H., Cha, J. J., Pasta, M., Koski, K. J., Yao, J., & Cui, Y. (2013) · Nano Letters · doi:10.1021/nl400258t · Cited by 2,250 · see citing works
Conducting MoS <sub>2</sub> Nanosheets as Catalysts for Hydrogen Evolution Reaction
Voiry, D., Salehi, M., Silva, R., Fujita, T., Chen, M., Asefa, T., Shenoy, V. B., Eda, G., & Chhowalla, M. (2013) · Nano Letters · doi:10.1021/nl403661s · Cited by 2,203 · see citing works
Catalyzing the hydrogen evolution reaction (HER) with molybdenum sulfide nanomaterials
Benck, J. D., Hellstern, T. R., Kibsgaard, J., Chakthranont, P., & Jaramillo, T. F. (2014) · ACS Catalysis · doi:10.1021/cs500923c · Cited by 1,617 · see citing works
Laursen, A. B., Kegnæs, S., Dahl, S., & Chorkendorff, I. (2012) · Energy & Environmental Science · doi:10.1039/c2ee02618j · Cited by 1,348 · see citing works
Amorphous molybdenum sulfide films as catalysts for electrochemical hydrogen production in water
Merki, D., Fierro, S., Vrubel, H., & Hu, X. (2011) · Chemical Science · doi:10.1039/c1sc00117e · Cited by 1,340 · see citing works
Faber, M. S., & Jin, S. (2014) · Energy Environ. Sci. · doi:10.1039/c4ee01760a · Cited by 1,317 · see citing works
Yin, Y., Han, J., Zhang, Y., Zhang, X., Xu, P., Yuan, Q., Samad, L., Wang, X., Wang, Y., Zhang, Z., et al. (2016) · Journal of the American Chemical Society · doi:10.1021/jacs.6b03714 · Cited by 1,263 · see citing works
A Molecular MoS <sub>2</sub> Edge Site Mimic for Catalytic Hydrogen Generation
Karunadasa, H. I., Montalvo, E., Sun, Y., Majda, M., Long, J. R., & Chang, C. J. (2012) · Science · doi:10.1126/science.1215868 · Cited by 1,215 · see citing works
Hopping transport through defect-induced localized states in molybdenum disulphide
Qiu, H., Xu, T., Wang, Z., Ren, W., Nan, H., Ni, Z., Chen, Q., Yuan, S., Miao, F., Song, F., et al. (2013) · Nature Communications · doi:10.1038/ncomms3642 · Cited by 1,190 · see citing works
Defects Engineered Monolayer MoS 2 for Improved Hydrogen Evolution Reaction
Ye, G., Gong, Y., Lin, J., Li, B., He, Y., Pantelides, S. T., Zhou, W., Vajtai, R., & Ajayan, P. M. (2016) · Nano Letters · doi:10.1021/acs.nanolett.5b04331 · Cited by 1,190 · see citing works
Recent developments of molybdenum and tungsten sulfides as hydrogen evolution catalysts
Merki, D., & Hu, X. (2011) · Energy & Environmental Science · doi:10.1039/c1ee01970h · Cited by 1,172 · see citing works
Chen, Z., Cummins, D., Reinecke, B. N., Clark, E., Sunkara, M. K., & Jaramillo, T. F. (2011) · Nano Letters · doi:10.1021/nl2020476 · Cited by 1,153 · see citing works
Benck, J. D., Chen, Z., Kuritzky, L. Y., Forman, A. J., & Jaramillo, T. F. (2012) · ACS Catalysis · doi:10.1021/cs300451q · Cited by 1,091 · see citing works
Wang, H., Lu, Z., Xu, S., Kong, D., Cha, J. J., Zheng, G. W., Hsu, P., Yan, K., Bradshaw, D., Prinz, F. B., et al. (2013) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1316792110 · Cited by 985 · see citing works
Controlled Scalable Synthesis of Uniform, High-Quality Monolayer and Few-layer MoS2 Films
Yu, Y., Li, C., Liu, Y., Su, L., Zhang, Y., & Cao, L. (2013) · Scientific Reports · doi:10.1038/srep01866 · Cited by 882 · see citing works
Self-citationTuning the MoS <sub>2</sub> Edge-Site Activity for Hydrogen Evolution via Support Interactions
Tsai, C., Abild-Pedersen, F., & Nørskov, J. K. (2014) · Nano Letters · doi:10.1021/nl404444k · Cited by 760 · see citing works
Gao, M.-R., Chan, M. K. Y., & Sun, Y. (2015) · Nature Communications · doi:10.1038/ncomms8493 · Cited by 736 · see citing works
Tsai, C., Chan, K., Abild-Pedersen, F., & Nørskov, J. K. (2014) · Phys. Chem. Chem. Phys. · doi:10.1039/c4cp01237b · Cited by 494 · see citing works
Gürarslan, A., Yu, Y., Su, L., Yu, Y., Suarez, F., Yao, S., Zhu, Y., Öztürk, M. C., Zhang, Y., & Cao, L. (2014) · ACS Nano · doi:10.1021/nn5057673 · Cited by 485 · see citing works
Self-citationShi, J., Ma, D., Han, G.-F., Zhang, Y., Ji, Q., Gao, T., Sun, J., Song, X., Li, C., Zhang, Y., et al. (2014) · ACS Nano · doi:10.1021/nn503211t · Cited by 459 · see citing works
Yu, Y., Hu, S., Su, L., et al. (2014) · Nano Letters · doi:10.1021/nl5038177 · Cited by 386 · see citing works
Self-citationTan, Y., Liu, P., Chen, L., Cong, W., Ito, Y., Han, J., Guo, X., Tang, Z., Fujita, T., Hirata, A., et al. (2014) · Advanced Materials · doi:10.1002/adma.201403808 · Cited by 329 · see citing works
Magnetic properties of MoS2: Existence of ferromagnetism
Tongay, S., Varnoosfaderani, S. S., Appleton, B. R., et al. (2012) · Applied Physics Letters · doi:10.1063/1.4753797 · Cited by 287 · see citing works
Cho, K., Min, M., Kim, T., et al. (2015) · ACS Nano · doi:10.1021/acsnano.5b04400 · Cited by 245 · see citing works
Tuning the Electronic and Magnetic Properties of MoS2 Nanoribbons by Strain Engineering
Pan, H., & Zhang, Y. (2012) · The Journal of Physical Chemistry C · doi:10.1021/jp3015782 · Cited by 234 · see citing works
Makarova, M. V., Okawa, Y., & Aono, M. (2012) · The Journal of Physical Chemistry C · doi:10.1021/jp307267h · Cited by 164 · see citing works
Li, Y., Yu, Y., Huang, Y., Nielsen, R. A., Goddard, W. A., Li, Y., & Cao, L. (2015) · ACS Catalysis · doi:10.1021/cs501635v · Cited by 155 · see citing works
Self-citationAtomically Thin MoS 2 Narrowband and Broadband Light Superabsorbers
Huang, L., Li, G., Gürarslan, A., et al. (2016) · ACS Nano · doi:10.1021/acsnano.6b02195 · Cited by 97 · see citing works
Self-citationTwo-dimensional transition-metal dichalcogenide materials: Toward an age of atomic-scale photonics
Cao, L. (2015) · MRS Bulletin · doi:10.1557/mrs.2015.144 · Cited by 68 · see citing works
Self-citation
Flagged first, then by citations
Research works printed but not linked: 6
- [10]10. Kong, D. et al. Synthesis of MoS2 and MoSe2 Films with Vertically Aligned Layers. Nano Letters 13, 1341-1347 (2013).
- [15]15. Voiry, D. et al. Conducting MoS2 Nanosheets as Catalysts for Hydrogen Evolution Reaction. Nano Letters 13, 6222-6227 (2013).
- [18]18. Yu, Y. et al. Layer-Dependent Electrocatalysis of MoS2 for Hydrogen Evolution. Nano Letters 14, 553-558 (2014).
- [28]28. Chen, Z.B. et al. Core-shell MoO3-MoS2 Nanowires for Hydrogen Evolution: A Functional Design for Electrocatalytic Materials. Nano Letters 11, 4168-4175 (2011).
- [32]32. Bockris, J.O. Pleskov's review of surface electrochemistry: A molecular level approach -Reply. Russ J Electrochem+ 31, 1211-1211 (1995).
- [36]36. Hinnemann, B. et al. Biornimetic hydrogen evolution: MoS2 nanoparticles as catalyst for hydrogen evolution. Journal of the American Chemical Society 127, 5308-5309 (2005).
Cited by
Sorted by citations
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Tian, X., Zhao, P., & Sheng, W. (2019) · Advanced Materials · doi:10.1002/adma.201808066 · Cited by 751 · see citing works
Zhang, X., Jia, F., & Song, S. (2021) · Chemical Engineering Journal · doi:10.1016/j.cej.2020.127013 · Cited by 145 · see citing works
Cheng, Y., Song, H., Wu, H., Zhang, P., Tang, Z., & Lu, S. (2020) · Chemistry – An Asian Journal · doi:10.1002/asia.202000752 · Cited by 86 · see citing works
Lei, L., Huang, D., Chen, Y., Chen, S., & Deng, R. (2021) · Journal of Materials Chemistry A · doi:10.1039/d1ta00505g · Cited by 54 · see citing works
Chandrasekaran, S., Feaster, J., Ynzunza, J., Li, F., Wang, X., Nelson, A. J., & Worsley, M. A. (2022) · ACS Materials Au · doi:10.1021/acsmaterialsau.2c00014 · Cited by 38 · see citing works
Non-equilibrium fractal growth of MoS <sub>2</sub> for electrocatalytic hydrogen evolution
Park, T., Bae, C., Lee, H., Leem, M., Kim, H., Ahn, W., Kim, J., Lee, E., Shin, H., & Kim, H. (2019) · CrystEngComm · doi:10.1039/c8ce01952e · Cited by 15 · see citing works
- Authors
- Li, G., Zhang, D., Qiao, Q., Yu, Y., Peterson, D., Zafar, A., Kumar, R., Curtarolo, S., Hunte, F., Shannon, S., Zhu, Y., Yang, W., & Cao, L.
- Affiliations
- North Carolina State University (US)
- Duke University (US)
- Brookhaven National Laboratory (US)
- Corresponding author
- Cao, Linyou
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-12-15
- Volume
- 138
- Issue
- 51
- Pages
- 16632-16638
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2558659093
- Cited by
- 829
- References
- 41
- Citations by year
- 2026: 48 · 2025: 68 · 2024: 76 · 2023: 79 · 2022: 95 · 2021: 98 · 2020: 107 · 2019: 123 · 2018: 85 · 2017: 49
- FWCI
- 23.21
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- Basic Energy Sciences (DE-SC0012575, DE-SC0012704)
- U.S. Department of Energy
- Division of Physics (PHY1338917)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › 2D Materials and Applications
- Physical Sciences › Engineering › Mechanical Engineering › Catalysis and Hydrodesulfurization Studies
- Keywords
- MoS2, hydrogen evolution reaction, catalytic site, sulfur vacancies, edge sites, grain boundaries, vacancy concentration, Tafel slope, crystal quality, electrocatalysis
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