We report here a theoretical study on 34 transition metal doped two-dimensional GaPS_(4) catalysts,denoted as transition metal transition metal@VS-GaPS_(4).Among them,the Pt@V_(S1)-GaPS_(4) single-atom catalyst is fou...We report here a theoretical study on 34 transition metal doped two-dimensional GaPS_(4) catalysts,denoted as transition metal transition metal@VS-GaPS_(4).Among them,the Pt@V_(S1)-GaPS_(4) single-atom catalyst is found to be stable with an ORR/OER overpotential of 0.59/0.41 V.Under the guidance of a volcano map,further biaxial strain engineering is adopted to tune the activity of Pt@V_(S1)-GaPS_(4) to the top of the volcano.The overpotentials of the OER/ORR are decreased to 0.37/0.33 V by applying a 3%tensile strain.Our results prove that Pt@V_(S1)-GaPS_(4) is an excellent candidate for OER/ORR bifunctional electro-catalysis.Moreover,bond angles and the highest occupied orbitals of the doped transition metal atoms can be used as descriptors to explain the underlying strain tunability mechanism.The machine learning method further predicts that the number of d electrons,the bond length and electronegativity are three main descriptors to determine the catalytic activity.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.12164009)which is received by Xuefei Liu+1 种基金the Guizhou Science and Technology Foundation-ZK[2022]General 308,which is received by Xuefei Liuand the Graduate Research Fund Project of Guizhou Province(YJSKYJJ[2021]088),which is received by Tianyun Liu.
文摘We report here a theoretical study on 34 transition metal doped two-dimensional GaPS_(4) catalysts,denoted as transition metal transition metal@VS-GaPS_(4).Among them,the Pt@V_(S1)-GaPS_(4) single-atom catalyst is found to be stable with an ORR/OER overpotential of 0.59/0.41 V.Under the guidance of a volcano map,further biaxial strain engineering is adopted to tune the activity of Pt@V_(S1)-GaPS_(4) to the top of the volcano.The overpotentials of the OER/ORR are decreased to 0.37/0.33 V by applying a 3%tensile strain.Our results prove that Pt@V_(S1)-GaPS_(4) is an excellent candidate for OER/ORR bifunctional electro-catalysis.Moreover,bond angles and the highest occupied orbitals of the doped transition metal atoms can be used as descriptors to explain the underlying strain tunability mechanism.The machine learning method further predicts that the number of d electrons,the bond length and electronegativity are three main descriptors to determine the catalytic activity.
