Chemical doping is a powerful method to intrinsically tailor the electrochemical properties of electrode materials.Here,an interstitial boron-doped tunnel-type VO_(2)(B)is constructed via a facile hydrothermal method....Chemical doping is a powerful method to intrinsically tailor the electrochemical properties of electrode materials.Here,an interstitial boron-doped tunnel-type VO_(2)(B)is constructed via a facile hydrothermal method.Various analysis techniques demonstrate that boron resides in the interstitial site of VO_(2)(B)and such interstitial doping can boost the zinc storage kinetics and structural stability of VO_(2)(B)cathode during cycling.Interestingly,we found that the boron doping level has a saturation limit peculiarity as proved by the quantitative analysis.Notably,the 2 at.%boron-doped VO_(2)(B)shows enhanced zinc ion storage performance with a high storage capacity of 281.7 mAh g^(-1) at 0.1 A g^(-1),excellent rate performance of 142.2 mAh g^(-1) at 20 A g^(-1),and long cycle stability up to 1000 cycles with the capacity retention of 133.3 mAh g^(-1) at 5 A g^(-1).Additionally,the successful preparation of the boron-doped tunneltype α-MnO_(2) further indicates that the interstitial boron doping approach is a general strategy,which supplies a new chance to design other types of functional electrode materials for multivalence batteries.展开更多
Single-atomic transition metal-nitrogen codoped carbon(M-N-C)are efficient substitute catalysts for noble metals to catalyze the electrochemical CO_(2) reduction reaction(CO_(2)RR).However,the uncontrolled aggregation...Single-atomic transition metal-nitrogen codoped carbon(M-N-C)are efficient substitute catalysts for noble metals to catalyze the electrochemical CO_(2) reduction reaction(CO_(2)RR).However,the uncontrolled aggregations of metal and serious loss of nitrogen species constituting the M-N_(x) active sites are frequently observed in the commonly used pyrolysis procedure.Herein,single-atomic nickel(Ni)-based sheet-like electrocatalysts with abundant Ni-N_(4) active sites were created by using a novel ammonium chloride(NH_(4)Cl)-assited pyrolysis method.Spherical aberration correction electron microscopy and X-ray absorption fine structure analysis clearly revealed that Ni species are atomically dispersed and anchored by N in Ni-N_(4) structure.The addition of NH_(4)Cl optimized the mesopore size to 7-10 nm and increased the concentrations of pyridinic N(3.54 wt%)and Ni-N_(4)(3.33 wt%)species.The synergistic catalytic effect derived from Ni-N_(4) active sites and pyridinic N species achieved an outstanding CO_(2) RR performance,presenting a high CO Faradaic efficiency(FE_(CO))up to 98% and a large CO partial current density of 8.5 mA cm^(-2) at a low potential of-0.62 V vs.RHE.Particularly,the FE_(CO) maintains above 80% within a large potential range from -0.43 to -0.73 V vs.RHE.This work provides a practical and feasible approach to building highly active single-atomic catalysts for CO_(2) conversion systems.展开更多
基金Key R&D projects of Henan Province,Grant/Award Number:221111240600National Natural Science Foundation of China,Grant/Award Numbers:U1704256,52272243,52202316+2 种基金Natural Science Foundation of Henan Province,Grant/Award Numbers:212300410300,212300410416PhD Research Fund Project,Grant/Award Number:13501050089School Key Project,Zhengzhou University of Light Industry,Grant/Award Number:2021ZDPY0203。
文摘Chemical doping is a powerful method to intrinsically tailor the electrochemical properties of electrode materials.Here,an interstitial boron-doped tunnel-type VO_(2)(B)is constructed via a facile hydrothermal method.Various analysis techniques demonstrate that boron resides in the interstitial site of VO_(2)(B)and such interstitial doping can boost the zinc storage kinetics and structural stability of VO_(2)(B)cathode during cycling.Interestingly,we found that the boron doping level has a saturation limit peculiarity as proved by the quantitative analysis.Notably,the 2 at.%boron-doped VO_(2)(B)shows enhanced zinc ion storage performance with a high storage capacity of 281.7 mAh g^(-1) at 0.1 A g^(-1),excellent rate performance of 142.2 mAh g^(-1) at 20 A g^(-1),and long cycle stability up to 1000 cycles with the capacity retention of 133.3 mAh g^(-1) at 5 A g^(-1).Additionally,the successful preparation of the boron-doped tunneltype α-MnO_(2) further indicates that the interstitial boron doping approach is a general strategy,which supplies a new chance to design other types of functional electrode materials for multivalence batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.21571159 and U1704256)the Natural Science Foundation of Henan Province,China(No.212300410299)the Doctoral Research Fund of Zhengzhou University of Light Industry(No.2018BSJJ024).
文摘Single-atomic transition metal-nitrogen codoped carbon(M-N-C)are efficient substitute catalysts for noble metals to catalyze the electrochemical CO_(2) reduction reaction(CO_(2)RR).However,the uncontrolled aggregations of metal and serious loss of nitrogen species constituting the M-N_(x) active sites are frequently observed in the commonly used pyrolysis procedure.Herein,single-atomic nickel(Ni)-based sheet-like electrocatalysts with abundant Ni-N_(4) active sites were created by using a novel ammonium chloride(NH_(4)Cl)-assited pyrolysis method.Spherical aberration correction electron microscopy and X-ray absorption fine structure analysis clearly revealed that Ni species are atomically dispersed and anchored by N in Ni-N_(4) structure.The addition of NH_(4)Cl optimized the mesopore size to 7-10 nm and increased the concentrations of pyridinic N(3.54 wt%)and Ni-N_(4)(3.33 wt%)species.The synergistic catalytic effect derived from Ni-N_(4) active sites and pyridinic N species achieved an outstanding CO_(2) RR performance,presenting a high CO Faradaic efficiency(FE_(CO))up to 98% and a large CO partial current density of 8.5 mA cm^(-2) at a low potential of-0.62 V vs.RHE.Particularly,the FE_(CO) maintains above 80% within a large potential range from -0.43 to -0.73 V vs.RHE.This work provides a practical and feasible approach to building highly active single-atomic catalysts for CO_(2) conversion systems.