Single MoTe2 sheet electrocatalytic microdevice for in situ revealing the activated basal plane sites by vacancies engineering
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Tianyou Zhai1(
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Activating basal plane inert sites will endow MoTe2 with prominent hydrogen evolution reaction (HER) catalytic capability and arouse a new family of HER catalysts. Herein, we fabricated single MoTe2 sheet electrocatalytic microdevice for in situ revealing the activated basal plane sites by vacancies introducing. Through the extraction of electrical parameters of single MoTe2 sheet, the in-plane and interlayer conductivities were optimized effectively by Te vacancies due to the defect levels. More deeply, Te vacancies can induce the delocalization of electrons around Mo atoms and shift the d-band center, as a consequence, facilitate the adsorption of H from the catalyst surface for HER catalysis. Benefiting by the coordinated regulation of band structure and local charge density, the overpotential at –10 mA∙cm−2 was reduced to 0.32 V after Te vacancies compared to 0.41 V for the basal plane sites of same MoTe2 nanosheet. Meanwhile, the insights gained from single nanosheet electrocatalytic microdevice can be applied to the improved HER of the commercial MoTe2 power. That the in situ testing of the atomic structure-electrical behavior-electrochemical properties of a single nanosheet before/after vacancies introducing provides reliable insight to structure-activity relationships.
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Single MoTe2 sheet electrocatalytic microdevice for in situ revealing the activated basal plane sites by vacancies engineering
), Tianyou Zhai1(
)
Abstract
Activating basal plane inert sites will endow MoTe2 with prominent hydrogen evolution reaction (HER) catalytic capability and arouse a new family of HER catalysts. Herein, we fabricated single MoTe2 sheet electrocatalytic microdevice for in situ revealing the activated basal plane sites by vacancies introducing. Through the extraction of electrical parameters of single MoTe2 sheet, the in-plane and interlayer conductivities were optimized effectively by Te vacancies due to the defect levels. More deeply, Te vacancies can induce the delocalization of electrons around Mo atoms and shift the d-band center, as a consequence, facilitate the adsorption of H from the catalyst surface for HER catalysis. Benefiting by the coordinated regulation of band structure and local charge density, the overpotential at –10 mA∙cm−2 was reduced to 0.32 V after Te vacancies compared to 0.41 V for the basal plane sites of same MoTe2 nanosheet. Meanwhile, the insights gained from single nanosheet electrocatalytic microdevice can be applied to the improved HER of the commercial MoTe2 power. That the in situ testing of the atomic structure-electrical behavior-electrochemical properties of a single nanosheet before/after vacancies introducing provides reliable insight to structure-activity relationships.
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Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (Nos. 21805102, 22071069, and 21825103), the Hubei Provincial Natural Science Foundation of China (No. 2019CFA002), and the Foundation of Basic and Applied Basic Research of Guangdong Province (No. 2019B1515120087). We also acknowledge technical support from Analytical and Testing Center in Huazhong University of Science and Technology.
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