Investigating Catalyst–Support Interactions To Improve the Hydrogen Evolution Reaction Activity of Thiomolybdate [Mo 3 S 13 ] 2– Nanoclusters
Abstract
Molybdenum sulfides have been identified as promising materials for catalyzing the hydrogen evolution reaction (HER) in acid, with active edge sites that exhibit some of the highest turnover frequencies among nonpreciousmetal catalysts. The thiomolybdate [Mo3S13]2- nanocluster catalyst contains a structural motif that resembles the active site of MoS2 and has been reported to be among the most active forms of molybdenum sulfide. Herein, we improve the activity of the [Mo3S13]2- catalysts through catalyst-support interactions. We synthesize [Mo3S13]2- on gold, silver, glassy carbon, and copper supports to demonstrate the ability to tune the hydrogen binding energy of [Mo3S13]2- using catalyst-support electronic interactions and optimize HER activity.
- Authors:
-
- Stanford Univ., CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States); Technical Univ. of Denmark, Lyngby (Denmark)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1426436
- Grant/Contract Number:
- AC02-76SF00515; EE006670; 9455; 1433442
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 10; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Hellstern, Thomas R., Kibsgaard, Jakob, Tsai, Charlie, Palm, David W., King, Laurie A., Abild-Pedersen, Frank, and Jaramillo, Thomas F. Investigating Catalyst–Support Interactions To Improve the Hydrogen Evolution Reaction Activity of Thiomolybdate [Mo 3 S 13 ] 2– Nanoclusters. United States: N. p., 2017.
Web. doi:10.1021/acscatal.7b02133.
Hellstern, Thomas R., Kibsgaard, Jakob, Tsai, Charlie, Palm, David W., King, Laurie A., Abild-Pedersen, Frank, & Jaramillo, Thomas F. Investigating Catalyst–Support Interactions To Improve the Hydrogen Evolution Reaction Activity of Thiomolybdate [Mo 3 S 13 ] 2– Nanoclusters. United States. https://doi.org/10.1021/acscatal.7b02133
Hellstern, Thomas R., Kibsgaard, Jakob, Tsai, Charlie, Palm, David W., King, Laurie A., Abild-Pedersen, Frank, and Jaramillo, Thomas F. Fri .
"Investigating Catalyst–Support Interactions To Improve the Hydrogen Evolution Reaction Activity of Thiomolybdate [Mo 3 S 13 ] 2– Nanoclusters". United States. https://doi.org/10.1021/acscatal.7b02133. https://www.osti.gov/servlets/purl/1426436.
@article{osti_1426436,
title = {Investigating Catalyst–Support Interactions To Improve the Hydrogen Evolution Reaction Activity of Thiomolybdate [Mo 3 S 13 ] 2– Nanoclusters},
author = {Hellstern, Thomas R. and Kibsgaard, Jakob and Tsai, Charlie and Palm, David W. and King, Laurie A. and Abild-Pedersen, Frank and Jaramillo, Thomas F.},
abstractNote = {Molybdenum sulfides have been identified as promising materials for catalyzing the hydrogen evolution reaction (HER) in acid, with active edge sites that exhibit some of the highest turnover frequencies among nonpreciousmetal catalysts. The thiomolybdate [Mo3S13]2- nanocluster catalyst contains a structural motif that resembles the active site of MoS2 and has been reported to be among the most active forms of molybdenum sulfide. Herein, we improve the activity of the [Mo3S13]2- catalysts through catalyst-support interactions. We synthesize [Mo3S13]2- on gold, silver, glassy carbon, and copper supports to demonstrate the ability to tune the hydrogen binding energy of [Mo3S13]2- using catalyst-support electronic interactions and optimize HER activity.},
doi = {10.1021/acscatal.7b02133},
journal = {ACS Catalysis},
number = 10,
volume = 7,
place = {United States},
year = {Fri Sep 22 00:00:00 EDT 2017},
month = {Fri Sep 22 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
Hydrogen production via solid electrolytic routes: Hydrogen production
journal, September 2012
- Badwal, Sukhvinder P. S.; Giddey, Sarbjit; Munnings, Christopher
- Wiley Interdisciplinary Reviews: Energy and Environment, Vol. 2, Issue 5
Photo-electrochemical hydrogen generation from water using solar energy. Materials-related aspects
journal, October 2002
- Bak, T.; Nowotny, J.; Rekas, M.
- International Journal of Hydrogen Energy, Vol. 27, Issue 10
Technical and economic feasibility of centralized facilities for solar hydrogen production via photocatalysis and photoelectrochemistry
journal, January 2013
- Pinaud, Blaise A.; Benck, Jesse D.; Seitz, Linsey C.
- Energy & Environmental Science, Vol. 6, Issue 7
Solar Water Splitting Cells
journal, November 2010
- Walter, Michael G.; Warren, Emily L.; McKone, James R.
- Chemical Reviews, Vol. 110, Issue 11, p. 6446-6473
Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices
journal, March 2015
- McCrory, Charles C. L.; Jung, Suho; Ferrer, Ivonne M.
- Journal of the American Chemical Society, Vol. 137, Issue 13
Recent Development in Hydrogen Evolution Reaction Catalysts and Their Practical Implementation
journal, March 2015
- Vesborg, Peter C. K.; Seger, Brian; Chorkendorff, Ib
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 6
Addressing the terawatt challenge: scalability in the supply of chemical elements for renewable energy
journal, January 2012
- Vesborg, Peter C. K.; Jaramillo, Thomas F.
- RSC Advances, Vol. 2, Issue 21
Evaluation of Pt, Ni, and Ni–Mo electrocatalysts for hydrogen evolution on crystalline Si electrodes
journal, January 2011
- McKone, James R.; Warren, Emily L.; Bierman, Matthew J.
- Energy & Environmental Science, Vol. 4, Issue 9
Ni–Mo Nanopowders for Efficient Electrochemical Hydrogen Evolution
journal, January 2013
- McKone, James R.; Sadtler, Bryce F.; Werlang, Caroline A.
- ACS Catalysis, Vol. 3, Issue 2
Molybdenum Boride and Carbide Catalyze Hydrogen Evolution in both Acidic and Basic Solutions
journal, November 2012
- Vrubel, Heron; Hu, Xile
- Angewandte Chemie International Edition, Vol. 51, Issue 51
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
Electrocatalytic hydrogen evolution using amorphous tungsten phosphide nanoparticles
journal, January 2014
- McEnaney, Joshua M.; Chance Crompton, J.; Callejas, Juan F.
- Chemical Communications, Vol. 50, Issue 75
Nanostructured Nickel Phosphide as an Electrocatalyst for the Hydrogen Evolution Reaction
journal, June 2013
- Popczun, Eric J.; McKone, James R.; Read, Carlos G.
- Journal of the American Chemical Society, Vol. 135, Issue 25
Highly Active Electrocatalysis of the Hydrogen Evolution Reaction by Cobalt Phosphide Nanoparticles
journal, April 2014
- Popczun, Eric J.; Read, Carlos G.; Roske, Christopher W.
- Angewandte Chemie, Vol. 126, Issue 21, p. 5531-5534
Engineering Cobalt Phosphide (CoP) Thin Film Catalysts for Enhanced Hydrogen Evolution Activity on Silicon Photocathodes
journal, December 2015
- Hellstern, Thomas R.; Benck, Jesse D.; Kibsgaard, Jakob
- Advanced Energy Materials, Vol. 6, Issue 4
An efficient molybdenum disulfide/cobalt diselenide hybrid catalyst for electrochemical hydrogen generation
journal, January 2015
- Gao, Min-Rui; Liang, Jin-Xia; Zheng, Ya-Rong
- Nature Communications, Vol. 6, Issue 1
Combining theory and experiment in electrocatalysis: Insights into materials design
journal, January 2017
- Seh, Zhi Wei; Kibsgaard, Jakob; Dickens, Colin F.
- Science, Vol. 355, Issue 6321
Hydrogen-Evolution Catalysts Based on Non-Noble Metal Nickel-Molybdenum Nitride Nanosheets
journal, May 2012
- Chen, Wei-Fu; Sasaki, Kotaro; Ma, Chao
- Angewandte Chemie International Edition, Vol. 51, Issue 25
Recent advances in transition metal phosphide nanomaterials: synthesis and applications in hydrogen evolution reaction
journal, January 2016
- Shi, Yanmei; Zhang, Bin
- Chemical Society Reviews, Vol. 45, Issue 6, p. 1529-1541
Catalyzing the Hydrogen Evolution Reaction (HER) with Molybdenum Sulfide Nanomaterials
journal, October 2014
- Benck, Jesse D.; Hellstern, Thomas R.; Kibsgaard, Jakob
- ACS Catalysis, Vol. 4, Issue 11
Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis
journal, October 2012
- Kibsgaard, Jakob; Chen, Zhebo; Reinecke, Benjamin N.
- Nature Materials, Vol. 11, Issue 11, p. 963-969
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
Amorphous Molybdenum Sulfide Catalysts for Electrochemical Hydrogen Production: Insights into the Origin of their Catalytic Activity
journal, August 2012
- Benck, Jesse D.; Chen, Zhebo; Kuritzky, Leah Y.
- ACS Catalysis, Vol. 2, Issue 9, p. 1916-1923
Fe, Co, and Ni ions promote the catalytic activity of amorphous molybdenum sulfide films for hydrogen evolution
journal, January 2012
- Merki, Daniel; Vrubel, Heron; Rovelli, Lorenzo
- Chemical Science, Vol. 3, Issue 8
Electrochemical Tuning of MoS 2 Nanoparticles on Three-Dimensional Substrate for Efficient Hydrogen Evolution
journal, April 2014
- Wang, Haotian; Lu, Zhiyi; Kong, Desheng
- ACS Nano, Vol. 8, Issue 5
Conducting MoS 2 Nanosheets as Catalysts for Hydrogen Evolution Reaction
journal, November 2013
- Voiry, Damien; Salehi, Maryam; Silva, Rafael
- Nano Letters, Vol. 13, Issue 12
Hydrogen Evolution on Supported Incomplete Cubane-type [Mo3S4]4+ Electrocatalysts
journal, November 2008
- Jaramillo, Thomas F.; Bonde, Jacob; Zhang, Jingdong
- The Journal of Physical Chemistry C, Vol. 112, Issue 45, p. 17492-17498
A Molecular MoS2 Edge Site Mimic for Catalytic Hydrogen Generation
journal, February 2012
- Karunadasa, H. I.; Montalvo, E.; Sun, Y.
- Science, Vol. 335, Issue 6069
Building an appropriate active-site motif into a hydrogen-evolution catalyst with thiomolybdate [Mo3S13]2− clusters
journal, January 2014
- Kibsgaard, Jakob; Jaramillo, Thomas F.; Besenbacher, Flemming
- Nature Chemistry, Vol. 6, Issue 3
Trends in the Exchange Current for Hydrogen Evolution
journal, January 2005
- Nørskov, J. K.; Bligaard, T.; Logadottir, A.
- Journal of The Electrochemical Society, Vol. 152, Issue 3
Modeling the Electrochemical Hydrogen Oxidation and Evolution Reactions on the Basis of Density Functional Theory Calculations
journal, October 2010
- Skúlason, Egill; Tripkovic, Vladimir; Björketun, Mårten E.
- The Journal of Physical Chemistry C, Vol. 114, Issue 42
Biomimetic Hydrogen Evolution: MoS 2 Nanoparticles as Catalyst for Hydrogen Evolution
journal, April 2005
- Hinnemann, Berit; Moses, Poul Georg; Bonde, Jacob
- Journal of the American Chemical Society, Vol. 127, Issue 15
Computational high-throughput screening of electrocatalytic materials for hydrogen evolution
journal, October 2006
- Greeley, Jeff; Jaramillo, Thomas F.; Bonde, Jacob
- Nature Materials, Vol. 5, Issue 11, p. 909-913
Designing an improved transition metal phosphide catalyst for hydrogen evolution using experimental and theoretical trends
journal, January 2015
- Kibsgaard, Jakob; Tsai, Charlie; Chan, Karen
- Energy & Environmental Science, Vol. 8, Issue 10
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
Co-Doped MoS 2 Nanosheets with the Dominant CoMoS Phase Coated on Carbon as an Excellent Electrocatalyst for Hydrogen Evolution
journal, December 2015
- Dai, Xiaoping; Du, Kangli; Li, Zhanzhao
- ACS Applied Materials & Interfaces, Vol. 7, Issue 49
Transition-metal doped edge sites in vertically aligned MoS2 catalysts for enhanced hydrogen evolution
journal, January 2015
- Wang, Haotian; Tsai, Charlie; Kong, Desheng
- Nano Research, Vol. 8, Issue 2
Rational design of MoS 2 catalysts: tuning the structure and activity via transition metal doping
journal, January 2015
- Tsai, Charlie; Chan, Karen; Nørskov, Jens K.
- Catalysis Science & Technology, Vol. 5, Issue 1
Tuning the MoS 2 Edge-Site Activity for Hydrogen Evolution via Support Interactions
journal, February 2014
- Tsai, Charlie; Abild-Pedersen, Frank; Nørskov, Jens K.
- Nano Letters, Vol. 14, Issue 3
Directed Synthesis of[Mo3S13]2−, an Isolated Cluster Containing Sulfur Atoms in Three Different States of Bonding
journal, July 1978
- Müller, Achim; Sarkar, Sabyasachi; Bhattacharyya, Ram Gopal
- Angewandte Chemie International Edition in English, Vol. 17, Issue 7
Spectroscopic investigation on the molecular and electronic structure of [Mo3S13]2−, a discrete binary transition metal sulfur cluster
journal, January 1980
- Müller, A.; Jostes, R.; Jaegermann, W.
- Inorganica Chimica Acta, Vol. 41
Identifying chemisorption in the interaction of thiol collectors with sulfide minerals by XPS: adsorption of xanthate on silver and silver sulfide
journal, November 1995
- Buckley, Alan N.; Woods, Ronald
- Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 104, Issue 2-3
XAS and XPS examination of the Au–S nanostructures produced via the reduction of aqueous gold(III) by sulfide ions
journal, February 2010
- Mikhlin, Yu.; Likhatski, M.; Tomashevich, Ye.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 177, Issue 1
ac Impedance of Faradaic reactions involving electrosorbed intermediates—I. Kinetic theory
journal, December 1987
- Harrington, D. A.; Conway, B. E.
- Electrochimica Acta, Vol. 32, Issue 12
Interfacial processes involving electrocatalytic evolution and oxidation of H2, and the role of chemisorbed H
journal, August 2002
- Conway, B. E.; Tilak, B. V.
- Electrochimica Acta, Vol. 47, Issue 22-23, p. 3571-3594
Behavior of overpotential—deposited species in Faradaic reactions—II. ac Impedance measurements on H2 evolution kinetics at activated and unactivated Pt cathodes
journal, December 1987
- Bai, Lijun; Harrington, D. A.; Conway, B. E.
- Electrochimica Acta, Vol. 32, Issue 12
Electrocatalysis of H2 evolution on RuO2 + IrO2 mixed oxide electrodes
journal, August 1994
- Kodintsev, I. M.; Trasatti, S.
- Electrochimica Acta, Vol. 39, Issue 11-12
Revealing and accelerating slow electron transport in amorphous molybdenum sulphide particles for hydrogen evolution reaction
journal, January 2013
- Vrubel, Heron; Moehl, Thomas; Grätzel, Michael
- Chemical Communications, Vol. 49, Issue 79
Hydrogen Evolution Over Bimetallic Systems: Understanding the Trends
journal, May 2006
- Greeley, Jeff; Nørskov, Jens K.; Kibler, Ludwig A.
- ChemPhysChem, Vol. 7, Issue 5, p. 1032-1035
Trends in the Hydrogen Evolution Activity of Metal Carbide Catalysts
journal, March 2014
- Michalsky, Ronald; Zhang, Yin-Jia; Peterson, Andrew A.
- ACS Catalysis, Vol. 4, Issue 5
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Works referencing / citing this record:
Nonprecious Intermetallic Al 7 Cu 4 Ni Nanocrystals Seamlessly Integrated in Freestanding Bimodal Nanoporous Copper for Efficient Hydrogen Evolution Catalysis
journal, January 2018
- Sun, Jie-Song; Wen, Zi; Han, Li-Ping
- Advanced Functional Materials, Vol. 28, Issue 14
State-of-the-Art Advances and Perspectives for Electrocatalysis
book, January 2020
- Ramohlola, Kabelo E.; Hato, Mpitloane J.; Monama, Gobeng R.
- Methods for Electrocatalysis: Advanced Materials and Allied Applications, p. 311-352
Tungsten-inert gas welding electrodes as low-cost, green and pH-universal electrocatalysts for the hydrogen evolution reaction
journal, January 2019
- Hashemniaye-Torshizi, Reihaneh; Ashraf, Narges; Arbab-Zavar, Mohammad Hossein
- New Journal of Chemistry, Vol. 43, Issue 29
Support and Interface Effects in Water‐Splitting Electrocatalysts
journal, December 2018
- Zhang, Jian; Zhang, Qiuyu; Feng, Xinliang
- Advanced Materials, Vol. 31, Issue 31
Gold nanoparticles as an outstanding catalyst for the hydrogen evolution reaction
journal, January 2018
- Tran, Tien D.; Nguyen, Mai T. T.; Le, Hoang V.
- Chemical Communications, Vol. 54, Issue 27
Nanostructured Nickel Nitride with Reduced Graphene Oxide Composite Bifunctional Electrocatalysts for an Efficient Water-Urea Splitting
journal, November 2019
- Wang, Feng; Zhao, Dongsheng; Zhang, Linbao
- Nanomaterials, Vol. 9, Issue 11
Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production
journal, January 2019
- Escalera-López, Daniel; Lou, Zhiheng; Rees, Neil V.
- Advanced Energy Materials, Vol. 9, Issue 8
Ni 1‐x Co x O y , Ni 1‐x Co x S y and Ni 1‐x Co x P y Catalysts Prepared from Ni 1‐x Co x ‐ZIF‐67 for Hydrogen Production by Electrolysis in Alkaline Media
journal, September 2019
- Cui, Yuchen; Liu, Zhi; Guo, Hailing
- ChemCatChem, Vol. 11, Issue 20
Hydrogen evolution reaction (HER) on Au@Ag ultrananoclusters as electro-catalysts
journal, January 2018
- Chang, Le; Cheng, Daojian; Sementa, Luca
- Nanoscale, Vol. 10, Issue 37
The mechanistic role of a support–catalyst interface in electrocatalytic water reduction by Co 3 O 4 supported nanocarbon florets
journal, January 2019
- Saha, Jayeeta; Ball, Ranadeb; Sah, Ananya
- Nanoscale, Vol. 11, Issue 28
Boosting the electrocatalytic activity of amorphous molybdenum sulfide nanoflakes via nickel sulfide decoration
journal, January 2019
- Zheng, Zheng; Su, Tong; Shi, Jianping
- Nanoscale, Vol. 11, Issue 47
The impact of microstructural features of carbon supports on the electrocatalytic hydrogen evolution reaction
journal, January 2019
- Suliman, Munzir H.; Adam, Alaaldin; Siddiqui, Mohammad N.
- Catalysis Science & Technology, Vol. 9, Issue 6
Polyoxothiometalate-Derivatized Silicon Photocathodes for Sunlight-Driven Hydrogen Evolution Reaction
journal, October 2018
- Fu, Dong; Fabre, Bruno; Loget, Gabriel
- ACS Omega, Vol. 3, Issue 10
Nanostructured Nickel Nitride with Reduced Graphene Oxide Composite Bifunctional Electrocatalysts for an Efficient Water-Urea Splitting
journal, November 2019
- Wang, Feng; Zhao, Dongsheng; Zhang, Linbao
- Nanomaterials, Vol. 9, Issue 11