摘要
Activating basal plane inert sites will endow MoTe_(2) with prominent hydrogen evolution reaction(HER)catalytic capability and arouse a new family of HER catalysts.Herein,we fabricated single MoTe_(2) sheet electrocatalytic microdevice for in situ revealing the activated basal plane sites by vacancies introducing.Through the extraction of electrical parameters of single MoTe_(2) 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 MoTe_(2) nanosheet.Meanwhile,the insights gained from single nanosheet electrocatalytic microdevice can be applied to the improved HER of the commercial MoTe_(2) 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.
基金
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)
the Foundation of Basic and Applied Basic Research of Guangdong Province(No.2019B1515120087)。
