Strong Interface Enhanced Hydrogen Evolution over Molybdenum-Based Catalysts
2020-06-22
发表期刊ACS APPLIED ENERGY MATERIALS
ISSN2574-0962
卷号3期号:6页码:5219-5228
发表状态已发表
DOI10.1021/acsaem.0c00045
摘要

By tuning interfacial structures, we have achieved an extremely small Tafel slope of 34.4 mV dec(-1) for the hydrogen evolution reaction (HER) over a molybdenum oxide catalyst in an acidic electrolyte. Such a small Tafel slope indicates the presence of active sites following the Volmer-Tafel mechanism, which is almost exclusively observed on platinum group metals. We attribute this excellent kinetic property to the enhancement effect from the metal/metal oxide Mo/MoOx) interface in the catalysts. This Mo/MoOx interface was obtained by tuning the hydrogen annealing method. Density functional theory calculations suggest that the hydrogen spillover from the Mo surface to the MoOx surface through an optimized interface will increase the hydrogen coverage on the MoOx surface. Thus, the hydrogen adsorption energy on MoOx can be reduced, making the recombination of the surface hydrogen feasible. Hydrogen temperature-programmed reduction provides clear evidence of hydrogen spillover from Mo to MoO2 at the Mo/MoO2 interfaces. Hence, the above Mo/MoOx interface will also lead to a high HER activity, as demonstrated by the high turnover frequency per active site (at 100, 150, and 200 mV vs the reversible hydrogen electrode, the values are approximately 0.004, 0.249, and 1.398 H-2 respectively). Our study demonstrates a new route to design low-cost-efficient HER catalysts of nonprecious metals by tuning transition metal/oxide interfaces.

关键词catalysis electrochemistry hydrogen evolution reaction molybdenum oxide metal/oxide interface
收录类别SCI ; SCIE ; EI
资助项目National Natural Science Foundation of China[11227902][21902103] ; Science and Technology Committee of Shanghai[14520722100] ; Certificate of China Postdoctoral Science Foundation[2015LH0031] ; ME2 project under National Natural Science Foundation of China[11227902]
WOS研究方向Chemistry ; Energy & Fuels ; Materials Science
WOS类目Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS记录号WOS:000543715100017
出版者AMER CHEMICAL SOC
WOS关键词INITIO MOLECULAR-DYNAMICS ; TOTAL-ENERGY CALCULATIONS ; MOS2 NANOSHEETS ; NICKEL PHOSPHIDE ; CARBON-DIOXIDE ; ELECTROCATALYST ; REDUCTION ; GRAPHENE ; PLANE ; MOO2
原始文献类型Article
引用统计
文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/122417
专题物质科学与技术学院_科学装置(X)_活细胞结构与功能成像等线站工程项目
物质科学与技术学院
大科学中心_PI研究组_刘志组
物质科学与技术学院_PI研究组_杨波组
物质科学与技术学院_硕士生
物质科学与技术学院_博士生
大科学中心
通讯作者Yang, Bo; Liu, Zhi; Li, Yimin
作者单位
1.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
2.Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Boston Coll, Dept Chem, Chestnut Hill, MA 02467 USA
第一作者单位物质科学与技术学院
通讯作者单位物质科学与技术学院
第一作者的第一单位物质科学与技术学院
推荐引用方式
GB/T 7714
Peng, Zheng,Wang, Kaili,Xu, Wei,et al. Strong Interface Enhanced Hydrogen Evolution over Molybdenum-Based Catalysts[J]. ACS APPLIED ENERGY MATERIALS,2020,3(6):5219-5228.
APA Peng, Zheng.,Wang, Kaili.,Xu, Wei.,Wang, Beibei.,Mao, Baohua.,...&Li, Yimin.(2020).Strong Interface Enhanced Hydrogen Evolution over Molybdenum-Based Catalysts.ACS APPLIED ENERGY MATERIALS,3(6),5219-5228.
MLA Peng, Zheng,et al."Strong Interface Enhanced Hydrogen Evolution over Molybdenum-Based Catalysts".ACS APPLIED ENERGY MATERIALS 3.6(2020):5219-5228.
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