The sluggish kinetics of the oxygen reduction reaction(ORR)and high over potential of oxygen evolution reaction(OER)are big challenges in the development of high-performance zinc-air batteries(ZABs)and fuel cells.In t...The sluggish kinetics of the oxygen reduction reaction(ORR)and high over potential of oxygen evolution reaction(OER)are big challenges in the development of high-performance zinc-air batteries(ZABs)and fuel cells.In this work,we report a rational design and a simple fabrication strategy of a photo-enhanced Co single-atom catalyst(SAC)comprising g-C3N4 coupled with cobalt-nitrogen-doped hierarchical mesoporous carbon(Co-N/MPC),forming a staggered p-n heterojunction that effectively improves charge separation and enhances electrocatalytic activity.The incorporation of Co SACs and g-C3N4 synergistically optimizes the photogenerated electron-hole pair separation,significantly boosting the intrinsic ORR-OER duplex activity.Under illumination,g-C_(3)N_(4)@Co-N/MPC exhibits an outstanding ORR half-wave potential(E1/2)of 0.841 V(vs.RHE)in 0.1 mol L^(–1)KOH and a low OER overpotential of 497.4 mV(vs.RHE)at 10 mA cm^(–2)in 1 mol L^(–1)KOH.Notably,the catalyst achieves an exceptional peak power density of 850.7 mW cm^(–2)in ZABs and of 411 mW cm^(–2)even in H_(2)-air fuel cell.In addition,g-C_(3)N_(4)@Co-N/MPC-based ZABs also show remarkable cycling stability exceeding 250 h.The advanced photo-induced charge separation at the p-n heterojunction facilitates faster electron transfer kinetics,and the mass transport owing to hierarchical mesoporous structure of Co-N-C,thereby reducing the overpotential and enhancing the overall energy conversion efficiency.This work provides a new perspective on designing next-generation of single-atom dispersed oxygen reaction catalysts,paving the way for high-performance photo-enhanced energy storage and conversion systems.展开更多
Chemodynamic therapy(CDT)offers a promising alternative to conventional cancer treatment.However,the limited acidity and H_(2)O_(2) concentration in tumor microenvironment(TME)severely impair the anticancer effects of...Chemodynamic therapy(CDT)offers a promising alternative to conventional cancer treatment.However,the limited acidity and H_(2)O_(2) concentration in tumor microenvironment(TME)severely impair the anticancer effects of CDT.In this study,we report a microemulsion-assisted coassembly method to prepare iron(III)tetraphenylporphyrin(FeTPP)and magnetic(Fe_(3)O_(4))nanocomposite material(FeTPP@Fe_(3)O_(4)),using photoactive FeTPP and Fe_(3)O_(4) nanocrystals as building blocks.The selfassembling nature of FeTPP results in disordered aggregation and fluorescence quenching,leading to a high light-to-heat conversion efficiency.Continuously,the photo-thermal effect enhances the catalytic decomposition of hydrogen peroxide(H_(2)O_(2))in the Fenton reaction on Fe_(3)O_(4) nanocrystals to generate highly toxic hydroxyl radicals(·OH)to destroy cancer cells.This cascade reaction produces a synergistic therapeutic effect between CDT and photothermal therapy(PTT),which significantly amplifies the therapeutic effect and enhances the treatment outcome of cancer patients.The highly efficient tumor catalytic therapy in vivo results confirmed that this nanomedicine treatment is an excellent biocompatible catalytic nanomedicine therapy achieved through a photo-enhanced Fenton reaction activity approach.展开更多
文摘The sluggish kinetics of the oxygen reduction reaction(ORR)and high over potential of oxygen evolution reaction(OER)are big challenges in the development of high-performance zinc-air batteries(ZABs)and fuel cells.In this work,we report a rational design and a simple fabrication strategy of a photo-enhanced Co single-atom catalyst(SAC)comprising g-C3N4 coupled with cobalt-nitrogen-doped hierarchical mesoporous carbon(Co-N/MPC),forming a staggered p-n heterojunction that effectively improves charge separation and enhances electrocatalytic activity.The incorporation of Co SACs and g-C3N4 synergistically optimizes the photogenerated electron-hole pair separation,significantly boosting the intrinsic ORR-OER duplex activity.Under illumination,g-C_(3)N_(4)@Co-N/MPC exhibits an outstanding ORR half-wave potential(E1/2)of 0.841 V(vs.RHE)in 0.1 mol L^(–1)KOH and a low OER overpotential of 497.4 mV(vs.RHE)at 10 mA cm^(–2)in 1 mol L^(–1)KOH.Notably,the catalyst achieves an exceptional peak power density of 850.7 mW cm^(–2)in ZABs and of 411 mW cm^(–2)even in H_(2)-air fuel cell.In addition,g-C_(3)N_(4)@Co-N/MPC-based ZABs also show remarkable cycling stability exceeding 250 h.The advanced photo-induced charge separation at the p-n heterojunction facilitates faster electron transfer kinetics,and the mass transport owing to hierarchical mesoporous structure of Co-N-C,thereby reducing the overpotential and enhancing the overall energy conversion efficiency.This work provides a new perspective on designing next-generation of single-atom dispersed oxygen reaction catalysts,paving the way for high-performance photo-enhanced energy storage and conversion systems.
基金supported by the National Natural Science Foundation of China(Nos.21802032,U21A2085,and 52102345)China Postdoctoral Science Foundation(No.2019TQ0081)+1 种基金Zhongyuan High Level Talents Special Support Plan(No.204200510009)Scientific and Technological Innovation Team in University of Henan Province(No.20IRTSTHN001).
文摘Chemodynamic therapy(CDT)offers a promising alternative to conventional cancer treatment.However,the limited acidity and H_(2)O_(2) concentration in tumor microenvironment(TME)severely impair the anticancer effects of CDT.In this study,we report a microemulsion-assisted coassembly method to prepare iron(III)tetraphenylporphyrin(FeTPP)and magnetic(Fe_(3)O_(4))nanocomposite material(FeTPP@Fe_(3)O_(4)),using photoactive FeTPP and Fe_(3)O_(4) nanocrystals as building blocks.The selfassembling nature of FeTPP results in disordered aggregation and fluorescence quenching,leading to a high light-to-heat conversion efficiency.Continuously,the photo-thermal effect enhances the catalytic decomposition of hydrogen peroxide(H_(2)O_(2))in the Fenton reaction on Fe_(3)O_(4) nanocrystals to generate highly toxic hydroxyl radicals(·OH)to destroy cancer cells.This cascade reaction produces a synergistic therapeutic effect between CDT and photothermal therapy(PTT),which significantly amplifies the therapeutic effect and enhances the treatment outcome of cancer patients.The highly efficient tumor catalytic therapy in vivo results confirmed that this nanomedicine treatment is an excellent biocompatible catalytic nanomedicine therapy achieved through a photo-enhanced Fenton reaction activity approach.
