Journal
CHEMICAL SCIENCE
Volume 11, Issue 13, Pages 3523-3530Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc00427h
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Funding
- North China Electric Power University
- Ministry of Business, Innovation and Employment [MAUX 1609]
- University of South Florida
- US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
- Office of Science of the US Department of Energy [DE-AC02-05CH11231]
- Australian Nuclear Science and Technology Organization (ANSTO)
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Optimizing interfacial contacts and thus electron transfer phenomena in heterogeneous electrocatalysts is an effective approach for enhancing electrocatalytic performance. Herein, we successfully synthesized ultrafine beta-Mo2C nanoparticles confined within hollow capsules of nitrogen-doped porous carbon (beta-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 beta-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 beta-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.
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