DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Atomically Precise Gold Nanoclusters Accelerate Hydrogen Evolution over MoS 2 Nanosheets: The Dual Interfacial Effect

Abstract

Abstract Hydrogen generation via electrocatalytic water splitting holds great promise for future energy revolution. It is desirable to design abundant and efficient catalysts and achieve mechanistic understanding of hydrogen evolution reaction (HER). Here, this paper reports a strategy for improving HER performance of molybdenum disulfide (MoS 2 ) via introducing gold nanoclusters as a cocatalyst. Compared to plain MoS 2 nanosheets, the Au 25 (SR) 18 /MoS 2 nanocomposite exhibits enhanced HER activity with a small onset potential of −0.20 V (vs reversible hydrogen electrode) and a higher current density of 59.3 mA cm −2 at the potential of −0.4 V. In addition to the interfacial interaction between nanoclusters and MoS 2 , the interface between the Au 25 core and the surface ligands (thiolate vs selenolate) is also discovered to distinctly affect the catalytic performance. This work highlights the promise of metal nanoclusters in boosting the HER performance via tailoring the interfacial electronic interactions between gold nanoclusters and MoS 2 nanosheets, as well as the interface between metal core and surface ligands.

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [1]
  1. Department of Chemistry Carnegie Mellon University Pittsburgh PA 15213 USA
  2. Chemical and Petroleum Engineering, and Physics University of Pittsburgh Pittsburgh PA 15261 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1401309
Grant/Contract Number:  
DE FG02‐03ER15476
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Name: Small Journal Volume: 13 Journal Issue: 43; Journal ID: ISSN 1613-6810
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Zhao, Shuo, Jin, Renxi, Song, Yongbo, Zhang, Hui, House, Stephen D., Yang, Judith C., and Jin, Rongchao. Atomically Precise Gold Nanoclusters Accelerate Hydrogen Evolution over MoS 2 Nanosheets: The Dual Interfacial Effect. Germany: N. p., 2017. Web. doi:10.1002/smll.201701519.
Zhao, Shuo, Jin, Renxi, Song, Yongbo, Zhang, Hui, House, Stephen D., Yang, Judith C., & Jin, Rongchao. Atomically Precise Gold Nanoclusters Accelerate Hydrogen Evolution over MoS 2 Nanosheets: The Dual Interfacial Effect. Germany. https://doi.org/10.1002/smll.201701519
Zhao, Shuo, Jin, Renxi, Song, Yongbo, Zhang, Hui, House, Stephen D., Yang, Judith C., and Jin, Rongchao. Mon . "Atomically Precise Gold Nanoclusters Accelerate Hydrogen Evolution over MoS 2 Nanosheets: The Dual Interfacial Effect". Germany. https://doi.org/10.1002/smll.201701519.
@article{osti_1401309,
title = {Atomically Precise Gold Nanoclusters Accelerate Hydrogen Evolution over MoS 2 Nanosheets: The Dual Interfacial Effect},
author = {Zhao, Shuo and Jin, Renxi and Song, Yongbo and Zhang, Hui and House, Stephen D. and Yang, Judith C. and Jin, Rongchao},
abstractNote = {Abstract Hydrogen generation via electrocatalytic water splitting holds great promise for future energy revolution. It is desirable to design abundant and efficient catalysts and achieve mechanistic understanding of hydrogen evolution reaction (HER). Here, this paper reports a strategy for improving HER performance of molybdenum disulfide (MoS 2 ) via introducing gold nanoclusters as a cocatalyst. Compared to plain MoS 2 nanosheets, the Au 25 (SR) 18 /MoS 2 nanocomposite exhibits enhanced HER activity with a small onset potential of −0.20 V (vs reversible hydrogen electrode) and a higher current density of 59.3 mA cm −2 at the potential of −0.4 V. In addition to the interfacial interaction between nanoclusters and MoS 2 , the interface between the Au 25 core and the surface ligands (thiolate vs selenolate) is also discovered to distinctly affect the catalytic performance. This work highlights the promise of metal nanoclusters in boosting the HER performance via tailoring the interfacial electronic interactions between gold nanoclusters and MoS 2 nanosheets, as well as the interface between metal core and surface ligands.},
doi = {10.1002/smll.201701519},
journal = {Small},
number = 43,
volume = 13,
place = {Germany},
year = {Mon Jul 24 00:00:00 EDT 2017},
month = {Mon Jul 24 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/smll.201701519

Citation Metrics:
Cited by: 70 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Near-Infrared Electrogenerated Chemiluminescence from Aqueous Soluble Lipoic Acid Au Nanoclusters
journal, May 2016

  • Wang, Tanyu; Wang, Dengchao; Padelford, Jonathan W.
  • Journal of the American Chemical Society, Vol. 138, Issue 20
  • DOI: 10.1021/jacs.6b03037

Three-Dimensional Hierarchical Frameworks Based on MoS 2 Nanosheets Self-Assembled on Graphene Oxide for Efficient Electrocatalytic Hydrogen Evolution
journal, November 2014

  • Zhou, Weijia; Zhou, Kai; Hou, Dongman
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 23
  • DOI: 10.1021/am506545g

Oxygen Electroreduction Catalyzed by Gold Nanoclusters: Strong Core Size Effects
journal, June 2009

  • Chen, Wei; Chen, Shaowei
  • Angewandte Chemie International Edition, Vol. 48, Issue 24, p. 4386-4389
  • DOI: 10.1002/anie.200901185

Enhanced Hydrogen Evolution Catalysis from Chemically Exfoliated Metallic MoS 2 Nanosheets
journal, May 2013

  • Lukowski, Mark A.; Daniel, Andrew S.; Meng, Fei
  • Journal of the American Chemical Society, Vol. 135, Issue 28
  • DOI: 10.1021/ja404523s

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
  • DOI: 10.1038/nmat1752

Edge-Specific Au/Ag Functionalization-Induced Conductive Paths in Armchair MoS 2 Nanoribbons
journal, September 2014

  • Li, Weifeng; Guo, Meng; Zhang, Gang
  • Chemistry of Materials, Vol. 26, Issue 19
  • DOI: 10.1021/cm5021756

One-pot synthesis of atomically monodisperse, thiol-functionalized Au 25 nanoclusters
journal, January 2009

  • Wu, Zhikun; Suhan, Joseph; Jin, Rongchao
  • J. Mater. Chem., Vol. 19, Issue 5
  • DOI: 10.1039/B815983A

Sustainable Hydrogen Production
journal, August 2004


Evolution from the plasmon to exciton state in ligand-protected atomically precise gold nanoparticles
journal, October 2016

  • Zhou, Meng; Zeng, Chenjie; Chen, Yuxiang
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13240

CO oxidation by MoS 2 -supported Au 19 nanoparticles: effects of vacancy formation and tensile strain
journal, January 2016

  • Kwon, Soonho; Shin, Kihyun; Bang, Kihoon
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 19
  • DOI: 10.1039/C6CP01100D

Recent progress in alkaline water electrolysis for hydrogen production and applications
journal, June 2010


Atomically Precise Gold Nanoclusters as New Model Catalysts
journal, March 2013

  • Li, Gao; Jin, Rongchao
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300213z

Ultrasmall Fe 3 O 4 Nanoparticle/MoS 2 Nanosheet Composites with Superior Performances for Lithium Ion Batteries
journal, December 2013


Structural patterns at all scales in a nonmetallic chiral Au 133 (SR) 52 nanoparticle
journal, March 2015

  • Zeng, Chenjie; Chen, Yuxiang; Kirschbaum, Kristin
  • Science Advances, Vol. 1, Issue 2
  • DOI: 10.1126/sciadv.1500045

Selective determination of dopamine using quantum-sized gold nanoparticles protected with charge selective ligands
journal, January 2012

  • Kwak, Kyuju; Kumar, S. Senthil; Lee, Dongil
  • Nanoscale, Vol. 4, Issue 14
  • DOI: 10.1039/c2nr30481c

Au25 Clusters as Electron-Transfer Catalysts Induced the Intramolecular Cascade Reaction of 2-nitrobenzonitrile
journal, November 2013

  • Chong, Hanbao; Li, Peng; Wang, Shuxin
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep03214

Pd coated MoS 2 nanoflowers for highly efficient hydrogen evolution reaction under irradiation
journal, June 2015


Mechanistic insights from atomically precise gold nanocluster-catalyzed reduction of 4-nitrophenol
journal, October 2016

  • Zhao, Shuo; Das, Anindita; Zhang, Hui
  • Progress in Natural Science: Materials International, Vol. 26, Issue 5
  • DOI: 10.1016/j.pnsc.2016.08.009

The Magic Au 60 Nanocluster: A New Cluster-Assembled Material with Five Au 13 Building Blocks
journal, May 2015

  • Song, Yongbo; Fu, Fangyu; Zhang, Jun
  • Angewandte Chemie International Edition, Vol. 54, Issue 29
  • DOI: 10.1002/anie.201501830

A Review of Photocatalysis using Self-organized TiO 2 Nanotubes and Other Ordered Oxide Nanostructures
journal, September 2012


Enhanced Electrocatalytic Properties of Transition-Metal Dichalcogenides Sheets by Spontaneous Gold Nanoparticle Decoration
journal, March 2013

  • Kim, Jaemyung; Byun, Segi; Smith, Alexander J.
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 8
  • DOI: 10.1021/jz400507t

Correlating the Crystal Structure of A Thiol-Protected Au25 Cluster and Optical Properties
journal, May 2008

  • Zhu, Manzhou; Aikens, Christine M.; Hollander, Frederick J.
  • Journal of the American Chemical Society, Vol. 130, Issue 18, p. 5883-5885
  • DOI: 10.1021/ja801173r

Gold Quantum Boxes: On the Periodicities and the Quantum Confinement in the Au 28 , Au 36 , Au 44 , and Au 52 Magic Series
journal, March 2016

  • Zeng, Chenjie; Chen, Yuxiang; Iida, Kenji
  • Journal of the American Chemical Society, Vol. 138, Issue 12
  • DOI: 10.1021/jacs.5b12747

Atomically precise metal nanoclusters: stable sizes and optical properties
journal, January 2015


Defect-Rich MoS 2 Ultrathin Nanosheets with Additional Active Edge Sites for Enhanced Electrocatalytic Hydrogen Evolution
journal, August 2013


Epitaxial Growth of Hetero-Nanostructures Based on Ultrathin Two-Dimensional Nanosheets
journal, September 2015

  • Tan, Chaoliang; Zhang, Hua
  • Journal of the American Chemical Society, Vol. 137, Issue 38
  • DOI: 10.1021/jacs.5b03590

Electrochemical tuning of vertically aligned MoS2 nanofilms and its application in improving hydrogen evolution reaction
journal, November 2013

  • Wang, H.; Lu, Z.; Xu, S.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 49
  • DOI: 10.1073/pnas.1316792110

Conversion of Anionic [Au 25 (SCH 2 CH 2 Ph) 18 ] Cluster to Charge Neutral Cluster via Air Oxidation
journal, July 2008

  • Zhu, Manzhou; Eckenhoff, William T.; Pintauer, Tomislav
  • The Journal of Physical Chemistry C, Vol. 112, Issue 37
  • DOI: 10.1021/jp805786p

Au Nanoparticle-Modified MoS 2 Nanosheet-Based Photoelectrochemical Cells for Water Splitting
journal, March 2014


Controllable Growth and Transfer of Monolayer MoS 2 on Au Foils and Its Potential Application in Hydrogen Evolution Reaction
journal, September 2014

  • Shi, Jianping; Ma, Donglin; Han, Gao-Feng
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn503211t

Photovoltaic Properties of Glutathione-Protected Gold Clusters Adsorbed on TiO 2 Electrodes
journal, June 2010


High-Performance Water Electrolysis System with Double Nanostructured Superaerophobic Electrodes
journal, March 2016


Plasmonic hot electron enhanced MoS 2 photocatalysis in hydrogen evolution
journal, January 2015

  • Kang, Yimin; Gong, Yongji; Hu, Zhijian
  • Nanoscale, Vol. 7, Issue 10
  • DOI: 10.1039/C4NR07303G

A molecule-like PtAu24(SC6H13)18 nanocluster as an electrocatalyst for hydrogen production
journal, March 2017

  • Kwak, Kyuju; Choi, Woojun; Tang, Qing
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14723

Atomically Precise Colloidal Metal Nanoclusters and Nanoparticles: Fundamentals and Opportunities
journal, September 2016


Crystal structure of Au 25 (SePh) 18 nanoclusters and insights into their electronic, optical and catalytic properties
journal, January 2014

  • Song, Yongbo; Zhong, Juan; Yang, Sha
  • Nanoscale, Vol. 6, Issue 22
  • DOI: 10.1039/C4NR04631E

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
  • DOI: 10.1126/science.1141483

Solution-phase epitaxial growth of noble metal nanostructures on dispersible single-layer molybdenum disulfide nanosheets
journal, February 2013

  • Huang, Xiao; Zeng, Zhiyuan; Bao, Shuyu
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2472

Emergence of hierarchical structural complexities in nanoparticles and their assembly
journal, December 2016


A Grand Avenue to Au Nanocluster Electrochemiluminescence
journal, January 2017


Ultrathin MoS 2 Nanoplates with Rich Active Sites as Highly Efficient Catalyst for Hydrogen Evolution
journal, December 2013

  • Yan, Ya; Xia, BaoYu; Ge, Xiaoming
  • ACS Applied Materials & Interfaces, Vol. 5, Issue 24
  • DOI: 10.1021/am404843b

Gold Nanoclusters Promote Electrocatalytic Water Oxidation at the Nanocluster/CoSe 2 Interface
journal, January 2017

  • Zhao, Shuo; Jin, Renxi; Abroshan, Hadi
  • Journal of the American Chemical Society, Vol. 139, Issue 3
  • DOI: 10.1021/jacs.6b12529

Hot Electron of Au Nanorods Activates the Electrocatalysis of Hydrogen Evolution on MoS 2 Nanosheets
journal, June 2015

  • Shi, Yi; Wang, Jiong; Wang, Chen
  • Journal of the American Chemical Society, Vol. 137, Issue 23
  • DOI: 10.1021/jacs.5b01732

Experimental and Computational Investigation of Au 25 Clusters and CO 2 : A Unique Interaction and Enhanced Electrocatalytic Activity
journal, June 2012

  • Kauffman, Douglas R.; Alfonso, Dominic; Matranga, Christopher
  • Journal of the American Chemical Society, Vol. 134, Issue 24
  • DOI: 10.1021/ja303259q

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
  • DOI: 10.1021/ja0504690