Probing the Crystal and Electronic Structures of Molybdenum Oxide in Redox Process: Implications for Energy Applications

被引:8
作者
Peng, Huayu [1 ,2 ]
Meng, Weiwei [1 ,2 ]
Zheng, He [1 ,2 ]
Wei, Yanjie [1 ,2 ]
Sheng, Huaping [1 ,2 ]
Liu, Huihui [1 ,2 ]
Li, Lei [1 ,2 ]
Wen, Guangyu [1 ,2 ]
Jia, Shuangfeng [1 ,2 ]
Li, Luying [3 ]
Wang, Jianbo [1 ,2 ]
机构
[1] Wuhan Univ, Sch Phys & Technol, Ctr Elect Microscopy, MOE Key Lab Artificial Micro & Nano Structures, Wuhan 430072, Peoples R China
[2] Wuhan Univ, Inst Adv Studies, Wuhan 430072, Peoples R China
[3] Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelectron, Ctr Nanoscale Characterizat Devices, Wuhan 430074, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
Mo nanoparticles; redox; core-shell structure; phase; valence state; electrocatalysis; HIGH-TEMPERATURE OXIDATION; THERMOELECTRIC PERFORMANCE; LOSS SPECTROSCOPY; PHASE EVOLUTION; SNO2; NANOWIRE; AES ANALYSES; OXYGEN; HYDROGEN; DYNAMICS; SURFACE;
D O I
10.1021/acsaem.9b01747
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Knowledge regarding the phase and valence state evolution of molybdenum (Mo) and its oxides during the redox reaction is essential for advancing their energy applications (e.g., electrocatalysis), which unfortunately remains largely unexplored. Herein, the effects of atomic and electronic structures on the electrocatalytic performance of Mo/oxides core-shell structures are investigated on the basis of the combination of ex situ and in situ experiments. First, a two-step reaction pathway is revealed during the oxidation of nanoscale Mo: the formation of amorphous MoO3 (A-MoO3) shells followed by the nucleation of crystalline alpha-MoO3. It is shown that the electrocatalytic performance of A-MoO3 is superior to that of alpha-MoO3, mainly due to more catalytically active sites in the former material. Furthermore, in situ transmission electron microscopy observations show that the A-MoO3 shell can be rapidly reduced into metallic MoO2 under reductive environment, which is likely to occur during the hydrogen evolution reaction measurement. Our in-depth characterization may contribute to the thorough and comprehensive understanding of the structural transition in Mo and its oxides during oxidative and reductive environments and thus serves as a reference for understanding the structure-property interplay for real energy applications.
引用
收藏
页码:7709 / 7716
页数:15
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