Engineering the local three-dimensional structure of metal sites has an important effect of maximizing the activity and selectivity of single-atom site catalysts.Here,we engineered a strain-assisted single Pt sites st...Engineering the local three-dimensional structure of metal sites has an important effect of maximizing the activity and selectivity of single-atom site catalysts.Here,we engineered a strain-assisted single Pt sites structure on a highly curved MoS_(2)surface to enhance its H_(2)S sensor property.By introducing N-methyl-2-pyrrolidone(NMP)as guiding molecules,a multilayer MoS_(2)structure with bending base planes was achieved.This bending behavior could inject not only uniform in-plane strain into the original inert MoS_(2)basal plane but also introduce sufficient accessible sites to anchor Pt monomers.Further experimental and theoretical results showed that the highcurvature MoS_(2)surface endowed 0.8%stretch strain onto the low-coordinated single Pt sites with a unique“tip”effect,which led to more accumulation of electrons around the Pt species,thereby accelerating the electric transfer process between H_(2)S and supports.The final catalyst delivered pronouncedly enhanced H_(2)S sensing response and response speed at room temperature.Our proposed strain-assisted strategy might create a new path to design highly active single-atom site catalysts for gas sensors.展开更多
基金This work was supported by the China Ministry of Science and Technology(grant no.2020YFA0710200)National Key R&D Program of China 2017YFA(grant nos.0208300 and 0700104)+2 种基金the National Natural Science Foundation of China(grant no.21671180)the Dalian National Laboratory for Clean Energy(DNL)Cooperation Fund,CAS(grant no.DNL201918)the Fundamental Research Funds for the Central Universities(grant nos.WK2060120004,WK2060000021,WK2060000025,and KY2060000180).
文摘Engineering the local three-dimensional structure of metal sites has an important effect of maximizing the activity and selectivity of single-atom site catalysts.Here,we engineered a strain-assisted single Pt sites structure on a highly curved MoS_(2)surface to enhance its H_(2)S sensor property.By introducing N-methyl-2-pyrrolidone(NMP)as guiding molecules,a multilayer MoS_(2)structure with bending base planes was achieved.This bending behavior could inject not only uniform in-plane strain into the original inert MoS_(2)basal plane but also introduce sufficient accessible sites to anchor Pt monomers.Further experimental and theoretical results showed that the highcurvature MoS_(2)surface endowed 0.8%stretch strain onto the low-coordinated single Pt sites with a unique“tip”effect,which led to more accumulation of electrons around the Pt species,thereby accelerating the electric transfer process between H_(2)S and supports.The final catalyst delivered pronouncedly enhanced H_(2)S sensing response and response speed at room temperature.Our proposed strain-assisted strategy might create a new path to design highly active single-atom site catalysts for gas sensors.
