Precise manipulation of atomic defects is essential for modulating the intrinsic properties of two-dimensional(2D)materials.In this study,sulfur(S)atoms are accurately knocked out in the 2D basal plane of pure tin dis...Precise manipulation of atomic defects is essential for modulating the intrinsic properties of two-dimensional(2D)materials.In this study,sulfur(S)atoms are accurately knocked out in the 2D basal plane of pure tin disulfide(SnS_(2)).By varying the annealing temperatures(250–350℃),SnS_(2)with different S vacancy concentrations(Vs-SnS_(2))can be obtained.When SnS_(2)is annealed at 350℃ for 5 h,the S vacancies in the forms of single S atom and double S atoms could reach up to 30.5%.The Vs-SnS_(2)is tested in the microelectrocatalytic hydrogen evolution reaction(HER).Vs-SnS_(2)with S vacancies of 30.5%generates superior catalytic performance,with a Tafel slope of 74 mV dec^(-1) and onset potential of 141 mV.The mechanism has been proposed.First,computation confirms that the absence of S atoms prompts surface charge modulation and enhances electronic conductivity.In addition,the under-coordinated Sn atoms adjacent to S vacancy introduce the lattice distortion and charge density redistribution,which are beneficial to hydrogen binding in HER.In short,accurate knockout of specific atoms by controlling the annealing temperature is a promising strategy to explore structure-dependent properties of various 2D materials.展开更多
基金supported by the National Natural Science Foundation of China(22175060 and 21975067)the Natural Science Foundation of Hunan Province,China(2021JJ10014 and 2021JJ30092)+4 种基金support from the National Natural Science Foundation of China(11974105)the National Basic Research Program of China(2016YFA0300901)support from the Natural Science Foundation of Jiangsu Province,China(BK20210729)the Collaborative Innovation Center of Suzhou Nano Science and Technologythe 111 Project and the Joint International Research Laboratory of Carbon-Based Functional Materials and Devices。
文摘Precise manipulation of atomic defects is essential for modulating the intrinsic properties of two-dimensional(2D)materials.In this study,sulfur(S)atoms are accurately knocked out in the 2D basal plane of pure tin disulfide(SnS_(2)).By varying the annealing temperatures(250–350℃),SnS_(2)with different S vacancy concentrations(Vs-SnS_(2))can be obtained.When SnS_(2)is annealed at 350℃ for 5 h,the S vacancies in the forms of single S atom and double S atoms could reach up to 30.5%.The Vs-SnS_(2)is tested in the microelectrocatalytic hydrogen evolution reaction(HER).Vs-SnS_(2)with S vacancies of 30.5%generates superior catalytic performance,with a Tafel slope of 74 mV dec^(-1) and onset potential of 141 mV.The mechanism has been proposed.First,computation confirms that the absence of S atoms prompts surface charge modulation and enhances electronic conductivity.In addition,the under-coordinated Sn atoms adjacent to S vacancy introduce the lattice distortion and charge density redistribution,which are beneficial to hydrogen binding in HER.In short,accurate knockout of specific atoms by controlling the annealing temperature is a promising strategy to explore structure-dependent properties of various 2D materials.
