Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the ...Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K_(0.5)Mn_(0.9)Mg_(0.025)Ti_(0.025)Al_(0.05)O_(2)cathode exhibited a discharge capacity of approximately 100 mA h g^(-1)at 20 mA g^(-1)with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g^(-1),showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.展开更多
Rechargeable metal-ion batteries, such as lithium-ion batteries(LIBs) and sodium-ion batteries(SIBs),have raised more attention because of the large demand for energy storage solutions. Undoubtedly, electrode material...Rechargeable metal-ion batteries, such as lithium-ion batteries(LIBs) and sodium-ion batteries(SIBs),have raised more attention because of the large demand for energy storage solutions. Undoubtedly, electrode materials and electrolytes are key parts of batteries, exhibiting critical influence on the reversible capacity and span life of the metal-ion battery. Nonetheless, researchers commonly express concerns regarding the stability of both electrodes and electrolytes. Given its commendable stability attributes,high-entropy materials have garnered widespread acclaim and have been applied in many fields since their inception, notably in energy storage. However, while certain high-entropy designs have achieved substantial breakthroughs, some have failed to meet anticipated outcomes within the high energy density energy storage materials. Moreover, there is a lack of comprehensive summary research on the corresponding mechanisms and design principles of high-entropy designs. This review examines the current high-entropy designs for cathodes, anodes, and electrolytes, aiming to summarize the design principle,potential mechanisms, and electrochemical performance. We focus on their structural characteristics,interface characteristics, and prospective development trends. At last, we provide a fair evaluation along-side succinct development suggestions.展开更多
基金financially supported by the National Natural Science Foundation of China(NSFC)(52274295)the Natural Science Foundation of Hebei Province(E2021501029)+3 种基金the Fundamental Research Funds for the Central Universities(N2423051,N2423053,N2302016,N2423019,N2323013,N2423005)the Science and Technology Project of Hebei Education Department(QN2024238)the Basic Research Program Project of Shijiazhuang City for Universities Stationed in Hebei Province(241790937A)the Science and Technology Project of Qinhuangdao City in 2023.
文摘Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K_(0.5)Mn_(0.9)Mg_(0.025)Ti_(0.025)Al_(0.05)O_(2)cathode exhibited a discharge capacity of approximately 100 mA h g^(-1)at 20 mA g^(-1)with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g^(-1),showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.
基金financially National Natural Science Foundation of China (NSFC) (52274295)Natural Science Foundation of Hebei Province (E2021501029, E2020501001, A2021501007, E2022501028, E2022501029)+11 种基金Natural Science Foundation - Steel and Iron Foundation of Hebei Province (No. E2022501030)Fundamental Research Funds for the Central Universities (No. N2323025, N2323013, N2302016, N2223009, N2223010, N2123035, N2023040)Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province (22567627H)Science and Technology Project of Hebei Education Department (ZD2022158)2023 Hebei Provincial doctoral candidate Innovation Ability training funding project (CXZZBS2023163)2023 Hebei Provincial Postgraduate Student Innovation Ability training funding project (CXZZSS2023195)Central Guided Local Science and Technology Development Fund Project of Hebei province (226Z4401G)The Fundamental Research Funds for the Central Universities (N2423052)Hebei Provincial Doctoral Candidate Innovation Ability Training Funding Project(CXZZBS2024176)The Science and Technology Project of Qinhuangdao City (202302B006)Science and Technology Project of Hebei Education Department (ZD2022158 and QN2024238)The Basic Research Project of Shijiazhuang City。
文摘Rechargeable metal-ion batteries, such as lithium-ion batteries(LIBs) and sodium-ion batteries(SIBs),have raised more attention because of the large demand for energy storage solutions. Undoubtedly, electrode materials and electrolytes are key parts of batteries, exhibiting critical influence on the reversible capacity and span life of the metal-ion battery. Nonetheless, researchers commonly express concerns regarding the stability of both electrodes and electrolytes. Given its commendable stability attributes,high-entropy materials have garnered widespread acclaim and have been applied in many fields since their inception, notably in energy storage. However, while certain high-entropy designs have achieved substantial breakthroughs, some have failed to meet anticipated outcomes within the high energy density energy storage materials. Moreover, there is a lack of comprehensive summary research on the corresponding mechanisms and design principles of high-entropy designs. This review examines the current high-entropy designs for cathodes, anodes, and electrolytes, aiming to summarize the design principle,potential mechanisms, and electrochemical performance. We focus on their structural characteristics,interface characteristics, and prospective development trends. At last, we provide a fair evaluation along-side succinct development suggestions.
