Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent tas...Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent task is to develop high-performance electrode materials and reveal their potassium storage mechanism.For PIBs anode materials,carbon with tunable microstructure,excellent electrochemical activity,nontoxicity and low price is considered as one of the most promising anode materials for commercialization.Although some breakthrough works have emerged,the overall electrochemical performance of the reported carbon anode is still far away from practical application.Herein,we carry out a comprehensive overview of PIBs carbon anode in terms of three aspects of rational design of structure,performance evaluation criteria and characterization of potassium storage mechanism.First,the regulation mechanism of key structural features of carbon anode on its potassium storage performance and the representative structural regulation strategies are introduced.Then,in view of the undefined performance evaluation criteria of PIBs carbon anode,a reference principle for evaluating the potassium storage performance of carbon anode is proposed.Finally,the advanced characterization techniques for the potassium storage mechanism of carbon anode are summarize.This review aims to provide guidance for the development of practical PIBs anode.展开更多
The electrocatalysis reactions involving oxygen,such as oxygen evolution reaction(OER)and oxygen reduction reaction(ORR),play a critical role in energy storage/conversion applications,e.g.,fuel cells,metal-air batteri...The electrocatalysis reactions involving oxygen,such as oxygen evolution reaction(OER)and oxygen reduction reaction(ORR),play a critical role in energy storage/conversion applications,e.g.,fuel cells,metal-air batteries,and electrochemical water splitting.The high kinetic energy barrier of the OER/ORR is highly associated with the spin state interconversion between singlet OH^(−)/H_(2)O and triplet O_(2),which is influenced by the spin state and magnetism of catalysts.This Review summarizes recent progress and advances in understanding spin/magnetism-related effects in oxygen electrocatalysis to develop spin theory.It is demonstrated that the spin states(low,intermediate,and high spin)of magnetic transition metal catalysts(TMCs)can directly affect the reaction barriers of OER/ORR by tailoring the bonding of oxygen intermediates with TMCs.Besides,the spin states of TMCs can build a spin-selective channel to filter the electron spins required for the single/triplet interconversion of O species during OER/ORR.In this Review,we introduced many approaches to modulating spin state,for instance,altering the crystal field,oxidation state of active-site ions,and the morphology of TMCs.What’s more,a magnetic field can drive the spin flip of magnetic ions to achieve the spin alignment(↑↑)(i.e.,facilitating spin polarization),which will strengthen the spin selectivity for accelerating the filtration and transfer of the spins with the same direction for the generation and conversion of triplet ↑O=O↑.Importantly,the origin of magnetic field enhancement on OER/ORR are deeply discussed,which provides a great vision for the magnetism-assisted catalysis.Finally,the challenges and perspectives for future development of spin/magnetism catalysis are presented.This Review is expected to highlight the significance of spin/magnetism theory in breaking the bottleneck of electrocatalysis field and promote the development of high-efficientcy electrocatalysts for practical applications.展开更多
基金supported financially by the National Key Research and Development Program of China (Grants No. 2017YFA0206301)the National Natural Science Foundation of China (Grants No. 51631001 and 51631001)the China-Germany Collaboration Project (Grants No. M-0199)
文摘Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent task is to develop high-performance electrode materials and reveal their potassium storage mechanism.For PIBs anode materials,carbon with tunable microstructure,excellent electrochemical activity,nontoxicity and low price is considered as one of the most promising anode materials for commercialization.Although some breakthrough works have emerged,the overall electrochemical performance of the reported carbon anode is still far away from practical application.Herein,we carry out a comprehensive overview of PIBs carbon anode in terms of three aspects of rational design of structure,performance evaluation criteria and characterization of potassium storage mechanism.First,the regulation mechanism of key structural features of carbon anode on its potassium storage performance and the representative structural regulation strategies are introduced.Then,in view of the undefined performance evaluation criteria of PIBs carbon anode,a reference principle for evaluating the potassium storage performance of carbon anode is proposed.Finally,the advanced characterization techniques for the potassium storage mechanism of carbon anode are summarize.This review aims to provide guidance for the development of practical PIBs anode.
基金supported by the National Natural Science Foundation of China(22222902,52027801,51871113,and 52111530236)the National Key R&D Program of China(2022YFA1203902 and 2022YFA1200093)the Natural Science Foundation of Jiangsu Province(BK20200047)。
基金financially supported by the National Natural Science Foundation of China(Grants No.52027801,52111530236)the National Postdoctoral Program for Innovative Talents(BX20220002)China Postdoctoral Science Foundation(2022M720204).
文摘The electrocatalysis reactions involving oxygen,such as oxygen evolution reaction(OER)and oxygen reduction reaction(ORR),play a critical role in energy storage/conversion applications,e.g.,fuel cells,metal-air batteries,and electrochemical water splitting.The high kinetic energy barrier of the OER/ORR is highly associated with the spin state interconversion between singlet OH^(−)/H_(2)O and triplet O_(2),which is influenced by the spin state and magnetism of catalysts.This Review summarizes recent progress and advances in understanding spin/magnetism-related effects in oxygen electrocatalysis to develop spin theory.It is demonstrated that the spin states(low,intermediate,and high spin)of magnetic transition metal catalysts(TMCs)can directly affect the reaction barriers of OER/ORR by tailoring the bonding of oxygen intermediates with TMCs.Besides,the spin states of TMCs can build a spin-selective channel to filter the electron spins required for the single/triplet interconversion of O species during OER/ORR.In this Review,we introduced many approaches to modulating spin state,for instance,altering the crystal field,oxidation state of active-site ions,and the morphology of TMCs.What’s more,a magnetic field can drive the spin flip of magnetic ions to achieve the spin alignment(↑↑)(i.e.,facilitating spin polarization),which will strengthen the spin selectivity for accelerating the filtration and transfer of the spins with the same direction for the generation and conversion of triplet ↑O=O↑.Importantly,the origin of magnetic field enhancement on OER/ORR are deeply discussed,which provides a great vision for the magnetism-assisted catalysis.Finally,the challenges and perspectives for future development of spin/magnetism catalysis are presented.This Review is expected to highlight the significance of spin/magnetism theory in breaking the bottleneck of electrocatalysis field and promote the development of high-efficientcy electrocatalysts for practical applications.
