Sluggish oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)kinetics inevitably impede the practical performance of rechargeable zinc-air batteries.Thus,combing the structural designability of transition ...Sluggish oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)kinetics inevitably impede the practical performance of rechargeable zinc-air batteries.Thus,combing the structural designability of transition metal-based electrocatalysts with anionic regulation is highly desired.Herein,mesoporous lamellar-stacked cobalt-based nanopiles with surface-sulfurization modification are elaborately designed and integrated with N/S co-doped graphene to build a robust OER/ORR bifunctional electrocatalyst.The lamellar-stacking mode of mesoporous nanosheets with abundant channels accelerates gas-liquid mass transfer,and partial-sulfurization of cobalt-based matrix surface efficiently improves the intrinsic OER activity.Meanwhile,N/S co-doped graphene further reinforces the ORR active sites while providing a stable conductive skeleton.As expected,this composite electrocatalyst delivers considerable bifunctional activity and stability,with an OER overpotential of 323 m V at 10 m A cm^(-2)and high durability.When applied in zinc-air batteries,remarkable ultralong-term stability over 4000 cycles and a maximum power density of 150.1 m W cm^(-2)are achieved.This work provides new insight into structurecomposition synergistic design of rapid-kinetics OER/ORR bifunctional electrocatalyst for nextgeneration metal-air batteries.展开更多
Photocatalytic oxidation techniques are promising for degradation of the highly ecotoxic and refractory isothiazolinone bactericides in relevant industrial wastewaters.However,low charge separation and directional tra...Photocatalytic oxidation techniques are promising for degradation of the highly ecotoxic and refractory isothiazolinone bactericides in relevant industrial wastewaters.However,low charge separation and directional transport efficiency under solar light radiation restrain their practical application.Here,we report a nanostructured photocatalyst doped with Gd and B in TiO_(2)with carbon incorporation and defect formation through incomplete calcination.The specific surface area,grain size,and hydrophilicity of TiO_(2)are improved,which is beneficial for the interfacial reaction between the photocatalyst and pollutants.The reduction of the bandgap,the broadening of the photo-absorption range,and the retarded electron-hole recombination promote the photocatalytic performance due to the improved oxygen vacancies based on the electron distribution modification.The difference in partial density of states(ΔPDOS)between the current catalyst and raw TiO_(2)indicates that the co-doping of Gd and B with incomplete calcination changes the electronic hybridization of conduction band and valence band near the Fermi level,and affects the band gap energy.It improved charge separation and directional transport efficiency and benefited the formation of main active species,including•OH and O2•−,for the pollutant decomposition.The rate of photocatalytic removal of benzisothiazolinone(BIT)by the current photocatalyst reaches 1.25 h^(−1),being 4.31 times that of TiO_(2).The current work offers a constructive approach to the design and synthesis of nanostructured photocatalysts for the photocatalytic degradation of refractory organic pollutants.展开更多
基金supported by the National Natural Science Foundation of China (21905157,22279077,21905056)the Hainan Provincial Natural Science Foundation of China (221RC452)+1 种基金the Start-up Research Foundation of Hainan University (KYQD (ZR)21059,KYQD (ZR)-21063)the Natural Science Foundation of Shanghai (22ZR1424500)。
文摘Sluggish oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)kinetics inevitably impede the practical performance of rechargeable zinc-air batteries.Thus,combing the structural designability of transition metal-based electrocatalysts with anionic regulation is highly desired.Herein,mesoporous lamellar-stacked cobalt-based nanopiles with surface-sulfurization modification are elaborately designed and integrated with N/S co-doped graphene to build a robust OER/ORR bifunctional electrocatalyst.The lamellar-stacking mode of mesoporous nanosheets with abundant channels accelerates gas-liquid mass transfer,and partial-sulfurization of cobalt-based matrix surface efficiently improves the intrinsic OER activity.Meanwhile,N/S co-doped graphene further reinforces the ORR active sites while providing a stable conductive skeleton.As expected,this composite electrocatalyst delivers considerable bifunctional activity and stability,with an OER overpotential of 323 m V at 10 m A cm^(-2)and high durability.When applied in zinc-air batteries,remarkable ultralong-term stability over 4000 cycles and a maximum power density of 150.1 m W cm^(-2)are achieved.This work provides new insight into structurecomposition synergistic design of rapid-kinetics OER/ORR bifunctional electrocatalyst for nextgeneration metal-air batteries.
基金the National Key R&D Program of China(No.2021YFC2102205)the National Natural Science Foundation of China(No.51808312)the CNNC Key Laboratory on Uranium Extraction from Seawater(No.KLUES202207).
文摘Photocatalytic oxidation techniques are promising for degradation of the highly ecotoxic and refractory isothiazolinone bactericides in relevant industrial wastewaters.However,low charge separation and directional transport efficiency under solar light radiation restrain their practical application.Here,we report a nanostructured photocatalyst doped with Gd and B in TiO_(2)with carbon incorporation and defect formation through incomplete calcination.The specific surface area,grain size,and hydrophilicity of TiO_(2)are improved,which is beneficial for the interfacial reaction between the photocatalyst and pollutants.The reduction of the bandgap,the broadening of the photo-absorption range,and the retarded electron-hole recombination promote the photocatalytic performance due to the improved oxygen vacancies based on the electron distribution modification.The difference in partial density of states(ΔPDOS)between the current catalyst and raw TiO_(2)indicates that the co-doping of Gd and B with incomplete calcination changes the electronic hybridization of conduction band and valence band near the Fermi level,and affects the band gap energy.It improved charge separation and directional transport efficiency and benefited the formation of main active species,including•OH and O2•−,for the pollutant decomposition.The rate of photocatalytic removal of benzisothiazolinone(BIT)by the current photocatalyst reaches 1.25 h^(−1),being 4.31 times that of TiO_(2).The current work offers a constructive approach to the design and synthesis of nanostructured photocatalysts for the photocatalytic degradation of refractory organic pollutants.
