Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfac...Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfacial interaction is achieved by epitaxial growth of high-quality N doped graphene(NG)on SiC(NG@SiC).This well-designed NG@SiC heterojunction demonstrates an intrinsic electric field with intensive interfacial interaction,making it an ideal prototype to thoroughly understand the configurations of electron/ion bridges and the mechanisms of interatomic electron migration.Both density functional theory(DFT)analysis and electrochemical kinetic analysis reveal that these intriguing electron/ion bridges can control and tailor the interfacial interaction via the interfacial coupled chemical bonds,enhancing the interfacial charge transfer kinetics and preventing pulverization/aggregation.As a proof-of-concept study,this well-designed NG@SiC anode shows good reversible capacity(1197.5 mAh g^(−1)after 200 cycles at 0.1 A g^(−1))and cycling durability with 76.6%capacity retention at 447.8 mAh g^(−1)after 1000 cycles at 10.0 A g^(−1).As expected,the lithium-ion full cell(LiFePO_(4)/C//NG@SiC)shows superior rate capability and cycling stability.This interfacial interaction tailoring strategy via epitaxial growth method provides new opportunities for traditional SiC-based anodes to achieve high-performance lithium-ion storage and beyond.展开更多
Electronic engineering of gallium nitride(Ga N) is critical for enhancement of its electrode performance.In this work, copper(Cu) cation substituted Ga N(Cu-Ga N) nanowires were fabricated to understand the electronic...Electronic engineering of gallium nitride(Ga N) is critical for enhancement of its electrode performance.In this work, copper(Cu) cation substituted Ga N(Cu-Ga N) nanowires were fabricated to understand the electronically engineered electrochemical performance for Li ion storage. Cu cation substitution was revealed at atomic level by combination of X-ray photoelectron spectroscopy(XPS), X-ray absorption fine structure(XAFS), density functional theory(DFT) simulation, and so forth. The Cu-Ga N electrode delivered high capacity of 813.2 m A h g^(-1) at 0.1 A g^(-1) after 200 cycles, increased by 66% relative to the unsubstituted Ga N electrode. After 2000 cycles at 10 A g^(-1),the reversible capacity was still maintained at326.7 m A h g^(-1). The DFT calculations revealed that Cu substitution introduced the impurity electronic states and efficient interatomic electron migration, which can enhance the charge transfer efficiency and reduce the Li ion adsorption energy on the Cu-Ga N electrode. The ex-situ SEM, TEM, HRTEM, and SAED analyses demonstrated the reversible intercalation Li ion storage mechanism and good structural stability. The concept of atomic-arrangement-assisted electronic engineering strategy is anticipated to open up opportunities for advanced energy storage applications.展开更多
基金supported by the National Natural Science Foundation of China(No.22074025)Guangzhou Municipal Science and Technology Project(No.202102010473)+5 种基金Science and Technology Program of Guangdong Province(2019B090905007)National Science Foundation of Guangdong Province(2021A1515010078)the Scientific and Technological Plan of Guangdong Province(2019B090905007)Natural Science Foundation of Shandong Province(Grant No.ZR2023QE059)China Postdoctoral Science Foundation(Grant No.2021M700915)Guangdong Basic and Applied Basic Research Foundation(2020A1515111086,2020A1515110219,and 2020A1515110770)for the financial support.
文摘Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfacial interaction is achieved by epitaxial growth of high-quality N doped graphene(NG)on SiC(NG@SiC).This well-designed NG@SiC heterojunction demonstrates an intrinsic electric field with intensive interfacial interaction,making it an ideal prototype to thoroughly understand the configurations of electron/ion bridges and the mechanisms of interatomic electron migration.Both density functional theory(DFT)analysis and electrochemical kinetic analysis reveal that these intriguing electron/ion bridges can control and tailor the interfacial interaction via the interfacial coupled chemical bonds,enhancing the interfacial charge transfer kinetics and preventing pulverization/aggregation.As a proof-of-concept study,this well-designed NG@SiC anode shows good reversible capacity(1197.5 mAh g^(−1)after 200 cycles at 0.1 A g^(−1))and cycling durability with 76.6%capacity retention at 447.8 mAh g^(−1)after 1000 cycles at 10.0 A g^(−1).As expected,the lithium-ion full cell(LiFePO_(4)/C//NG@SiC)shows superior rate capability and cycling stability.This interfacial interaction tailoring strategy via epitaxial growth method provides new opportunities for traditional SiC-based anodes to achieve high-performance lithium-ion storage and beyond.
基金supported by the National Natural Science Foundation of China(51672144,51572137,5170218121905152,52072196,52002199,52002200)the Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09)+5 种基金the Shandong Provincial Key Research and Development Program(SPKR&DP)(2019GGX102055)the Natural Science Foundation of Shandong Province(ZR2019BEM042 ZR2020QE063,ZR2020MB045)the Innovation and Technology Program of Shandong Province(2020KJA004)the Innovation Pilot Project of Integration of Science,Education and Industry of Shandong Province(2020KJC-CG04)the Guangdong Basic and Applied Basic Research Foundation(019A15151109332020A1515111086,2020A1515110219)the Shandong Provincial Universities Young Innovative Talent Incubation ProgramInorganic Non-metallic Materials Research and Innovation Team,and Taishan Scholars Program of Shandong Province(ts201511034)。
文摘Electronic engineering of gallium nitride(Ga N) is critical for enhancement of its electrode performance.In this work, copper(Cu) cation substituted Ga N(Cu-Ga N) nanowires were fabricated to understand the electronically engineered electrochemical performance for Li ion storage. Cu cation substitution was revealed at atomic level by combination of X-ray photoelectron spectroscopy(XPS), X-ray absorption fine structure(XAFS), density functional theory(DFT) simulation, and so forth. The Cu-Ga N electrode delivered high capacity of 813.2 m A h g^(-1) at 0.1 A g^(-1) after 200 cycles, increased by 66% relative to the unsubstituted Ga N electrode. After 2000 cycles at 10 A g^(-1),the reversible capacity was still maintained at326.7 m A h g^(-1). The DFT calculations revealed that Cu substitution introduced the impurity electronic states and efficient interatomic electron migration, which can enhance the charge transfer efficiency and reduce the Li ion adsorption energy on the Cu-Ga N electrode. The ex-situ SEM, TEM, HRTEM, and SAED analyses demonstrated the reversible intercalation Li ion storage mechanism and good structural stability. The concept of atomic-arrangement-assisted electronic engineering strategy is anticipated to open up opportunities for advanced energy storage applications.
