Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo2C nanostructures,Chemical Science

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Highly efficient electrocatalytic hydrogen evolution promoted by O–Mo–C interfaces of ultrafine β-Mo2C nanostructures
Chemical Science ( IF 7.6 ) Pub Date : 2020/03/12 , DOI: 10.1039/d0sc00427h
Hui Yang _{1,

2} , Xing Chen ₃ , Guoxiang Hu ₄ , Wan-Ting Chen ₅ , Siobhan J Bradley ₆ , Weijie Zhang ₂ , Gaurav Verma ₂ , Thomas Nann ₆ , De-En Jiang ₇ , Paul E Kruger ₈ , Xiangke Wang ₁ , He Tian ₃ , Geoffrey I N Waterhouse ₅ , Shane G Telfer ₉ , Shengqian Ma ₂

Affiliation

College of Environmental Science and Engineering, North China Electric Power University Beijing 102206 P. R. China
Department of Chemistry, University of South Florida 4202 E. Fowler Avenue Tampa Florida 33620 USA
Center of Electron Microscopy, Zhejiang University Hangzhou 310027 P. R. China
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory Oak Ridge Tennessee 37831 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 California Riverside California 92521 USA.
MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Physical and Chemical Sciences, University of Canterbury Christchurch 8140 New Zealand.
MacDiarmid Institute for Advanced Materials and Nanotechnology, Institute of Fundamental Sciences, Massey University Palmerston North 4442 New Zealand.

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.

中文翻译：

超细β-Mo2C纳米结构的O-Mo-C界面促进高效电催化析氢

优化多相电催化剂中的界面接触和电子转移现象是提高电催化性能的有效方法。在此，我们成功合成了限制在氮掺杂多孔碳空心胶囊内的超细β-Mo ₂ C纳米粒子（β-Mo ₂ C@NPCC），并发现钼原子的表面层被进一步氧化为单个Mo-O表面层，从而产生紧密的O-Mo-C界面。一系列互补技术，包括 XPS、原子分辨率 HAADF-STEM 和 XAS 分析，清楚地揭示了这些表面工程超细纳米结构的 O-Mo-C 界面的存在。β-Mo ₂ C@NPCC电催化剂对水中的析氢反应（HER）表现出优异的电催化活性。_{理论研究表明，作为活性位点的易接近的超薄O-Mo-C界面对于HER性能至关重要，并支撑了β-Mo 2} C @NPCC出色的电催化性能。这项概念验证研究为 HER 和其他应用的高效催化剂的制造开辟了一条新途径，同时进一步证明了暴露界面和界面接触在高效电催化中的重要性。

更新日期：2020-04-01

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