Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo 2 C nanostructures
Abstract
Optimizing interfacial contacts and thus electron transfer phenomena in heterogeneous electrocatalysts is an effective approach for enhancing electrocatalytic performance. Herein, we successfully synthesized ultrafine β-Mo2C nanoparticles confined within hollow capsules of nitrogen-doped porous carbon (β-Mo2C@NPCC) and found that the surface layer of molybdenum atoms was further oxidized to a single Mo–O surface layer, thus producing intimate O–Mo–C interfaces. An arsenal of complementary technologies, including XPS, atomic-resolution HAADF-STEM, and XAS analysis clearly reveals the existence of O–Mo–C interfaces for these surface-engineered ultrafine nanostructures. The β-Mo2C@NPCC electrocatalyst exhibited excellent electrocatalytic activity for the hydrogen evolution reaction (HER) in water. Theoretical studies indicate that the highly accessible ultrathin O–Mo–C interfaces serving as the active sites are crucial to the HER performance and underpinned the outstanding electrocatalytic performance of β-Mo2C@NPCC. This proof-of-concept study opens a new avenue for the fabrication of highly efficient catalysts for HER and other applications, whilst further demonstrating the importance of exposed interfaces and interfacial contacts in efficient electrocatalysis.
- Authors:
-
[7];
[8];
[9];
[10];
[6]
- College of Environmental Science and Engineering, North China Electric Power University, Beijing, P. R. China, Department of Chemistry
- Center of Electron Microscopy, Zhejiang University, Hangzhou 310027, P. R. China
- Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, USA
- MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical Sciences, The University of Auckland, Auckland 1142, New Zealand
- MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington 6140, New Zealand
- Department of Chemistry, University of South Florida, Tampa, USA
- Department of Chemistry, University of California, Riverside, USA
- MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Physical and Chemical Sciences, University of Canterbury, Christchurch 8140, New Zealand
- College of Environmental Science and Engineering, North China Electric Power University, Beijing, P. R. China
- MacDiarmid Institute for Advanced Materials and Nanotechnology, Institute of Fundamental Sciences, Massey University, Palmerston North 4442, New Zealand
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Ministry of Business, Innovation and Employment
- OSTI Identifier:
- 1604219
- Alternate Identifier(s):
- OSTI ID: 1809998
- Grant/Contract Number:
- AC02-05CH11231; AC05-00OR22725; MAUX-1609
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 11 Journal Issue: 13; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Yang, Hui, Chen, Xing, Hu, Guoxiang, Chen, Wan-Ting, Bradley, Siobhan J., Zhang, Weijie, Verma, Gaurav, Nann, Thomas, Jiang, De-en, Kruger, Paul E., Wang, Xiangke, Tian, He, Waterhouse, Geoffrey I. N., Telfer, Shane G., and Ma, Shengqian. Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo 2 C nanostructures. United Kingdom: N. p., 2020.
Web. doi:10.1039/D0SC00427H.
Yang, Hui, Chen, Xing, Hu, Guoxiang, Chen, Wan-Ting, Bradley, Siobhan J., Zhang, Weijie, Verma, Gaurav, Nann, Thomas, Jiang, De-en, Kruger, Paul E., Wang, Xiangke, Tian, He, Waterhouse, Geoffrey I. N., Telfer, Shane G., & Ma, Shengqian. Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo 2 C nanostructures. United Kingdom. https://doi.org/10.1039/D0SC00427H
Yang, Hui, Chen, Xing, Hu, Guoxiang, Chen, Wan-Ting, Bradley, Siobhan J., Zhang, Weijie, Verma, Gaurav, Nann, Thomas, Jiang, De-en, Kruger, Paul E., Wang, Xiangke, Tian, He, Waterhouse, Geoffrey I. N., Telfer, Shane G., and Ma, Shengqian. Wed .
"Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo 2 C nanostructures". United Kingdom. https://doi.org/10.1039/D0SC00427H.
@article{osti_1604219,
title = {Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo 2 C nanostructures},
author = {Yang, Hui and Chen, Xing and Hu, Guoxiang and Chen, Wan-Ting and Bradley, Siobhan J. and Zhang, Weijie and Verma, Gaurav and Nann, Thomas and Jiang, De-en and Kruger, Paul E. and Wang, Xiangke and Tian, He and Waterhouse, Geoffrey I. N. and Telfer, Shane G. and Ma, Shengqian},
abstractNote = {Optimizing interfacial contacts and thus electron transfer phenomena in heterogeneous electrocatalysts is an effective approach for enhancing electrocatalytic performance. Herein, we successfully synthesized ultrafine β-Mo2C nanoparticles confined within hollow capsules of nitrogen-doped porous carbon (β-Mo2C@NPCC) and found that the surface layer of molybdenum atoms was further oxidized to a single Mo–O surface layer, thus producing intimate O–Mo–C interfaces. An arsenal of complementary technologies, including XPS, atomic-resolution HAADF-STEM, and XAS analysis clearly reveals the existence of O–Mo–C interfaces for these surface-engineered ultrafine nanostructures. The β-Mo2C@NPCC electrocatalyst exhibited excellent electrocatalytic activity for the hydrogen evolution reaction (HER) in water. Theoretical studies indicate that the highly accessible ultrathin O–Mo–C interfaces serving as the active sites are crucial to the HER performance and underpinned the outstanding electrocatalytic performance of β-Mo2C@NPCC. This proof-of-concept study opens a new avenue for the fabrication of highly efficient catalysts for HER and other applications, whilst further demonstrating the importance of exposed interfaces and interfacial contacts in efficient electrocatalysis.},
doi = {10.1039/D0SC00427H},
journal = {Chemical Science},
number = 13,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {4}
}
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