{"title":"嵌入 N 和 S 共掺杂多孔碳正极中的 Li3V2(PO4)3 粒子用于高性能锂存储:实验和 DFT 研究","authors":"Jinggao Wu, Canyu Zhong, Xiaofan Chen, Jing Huang","doi":"10.1039/d4qi01916d","DOIUrl":null,"url":null,"abstract":"Li3V2(PO4)3 (LVP)-coated with N and S co-doped carbon (NSC) is investigated by DFT calculation, suggesting that NSC significantly enhances electronic conductivity and lowers Li+ migration energy barrier in comparison to the LVP-embeded pristine carbon. To experimentally confirm the theoretical prediction, three types of LVP particles embedded N and S co-doped porous carbon (LVP@NSC) materials with various nitrogen and sulfur molar ratios (N:S=1:1, 1:2 and 2:1) were prepared by a facile freeze drying-assisted wet chemical route associated with a post-annealing process. When using as a cathode for lithium-ion battery (LIB), the designed LVP@NSC with N:S=1:2 exhibits outstanding high rate capacities of 124.4 and 107.85 mA h g-1 at 2 and 20 C in a voltage window of 3.0-4.3 V, respectively, and a ultralong cycle stability of 500 times at 20 C with remaining a reversible capacity of 100.22 mA h g−1 possibly due to its smallest charge transfer resistance and highest Li+ migration coefficiency, which is in good agreement with the theoretical rediction. This work not only reveals the critical role of interaction mechanism between NSC and LVP, but also offers great potentials for high energy density LIBs applications.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"246 1","pages":""},"PeriodicalIF":6.1000,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Li3V2(PO4)3 particles embedded in N and S Co-doped porous carbon cathode for high performance lithium storage:An experimental and DFT study\",\"authors\":\"Jinggao Wu, Canyu Zhong, Xiaofan Chen, Jing Huang\",\"doi\":\"10.1039/d4qi01916d\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Li3V2(PO4)3 (LVP)-coated with N and S co-doped carbon (NSC) is investigated by DFT calculation, suggesting that NSC significantly enhances electronic conductivity and lowers Li+ migration energy barrier in comparison to the LVP-embeded pristine carbon. To experimentally confirm the theoretical prediction, three types of LVP particles embedded N and S co-doped porous carbon (LVP@NSC) materials with various nitrogen and sulfur molar ratios (N:S=1:1, 1:2 and 2:1) were prepared by a facile freeze drying-assisted wet chemical route associated with a post-annealing process. When using as a cathode for lithium-ion battery (LIB), the designed LVP@NSC with N:S=1:2 exhibits outstanding high rate capacities of 124.4 and 107.85 mA h g-1 at 2 and 20 C in a voltage window of 3.0-4.3 V, respectively, and a ultralong cycle stability of 500 times at 20 C with remaining a reversible capacity of 100.22 mA h g−1 possibly due to its smallest charge transfer resistance and highest Li+ migration coefficiency, which is in good agreement with the theoretical rediction. This work not only reveals the critical role of interaction mechanism between NSC and LVP, but also offers great potentials for high energy density LIBs applications.\",\"PeriodicalId\":79,\"journal\":{\"name\":\"Inorganic Chemistry Frontiers\",\"volume\":\"246 1\",\"pages\":\"\"},\"PeriodicalIF\":6.1000,\"publicationDate\":\"2024-11-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganic Chemistry Frontiers\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1039/d4qi01916d\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry Frontiers","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d4qi01916d","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0
摘要
通过 DFT 计算研究了包覆有 N 和 S 共掺杂碳(NSC)的 Li3V2(PO4)3(LVP),结果表明,与嵌入 LVP 的原始碳相比,NSC 能显著增强电子导电性并降低 Li+ 迁移能垒。为了在实验中证实这一理论预测,研究人员采用一种简便的冷冻干燥辅助湿化学方法,并结合一种后退火工艺,制备了三种嵌入 N 和 S 共掺多孔碳(LVP@NSC)的 LVP 粒子材料,其氮、硫摩尔比各不相同(N:S=1:1、1:2 和 2:1)。当用作锂离子电池(LIB)正极时,所设计的 N:S=1:2 的 LVP@NSC 在 3.0-4.3 V 的电压窗口内,分别于 2 C 和 20 C 条件下表现出 124.4 和 107.85 mA h g-1 的出色高倍率容量,并且在 20 C 条件下具有 500 次的超长循环稳定性,剩余可逆容量为 100.22 mA h g-1,这可能是由于它具有最小的电荷转移电阻和最高的 Li+ 迁移系数,这与理论预测结果非常吻合。这项研究不仅揭示了 NSC 与 LVP 之间相互作用机制的关键作用,还为高能量密度锂离子电池的应用提供了巨大潜力。
Li3V2(PO4)3 particles embedded in N and S Co-doped porous carbon cathode for high performance lithium storage:An experimental and DFT study
Li3V2(PO4)3 (LVP)-coated with N and S co-doped carbon (NSC) is investigated by DFT calculation, suggesting that NSC significantly enhances electronic conductivity and lowers Li+ migration energy barrier in comparison to the LVP-embeded pristine carbon. To experimentally confirm the theoretical prediction, three types of LVP particles embedded N and S co-doped porous carbon (LVP@NSC) materials with various nitrogen and sulfur molar ratios (N:S=1:1, 1:2 and 2:1) were prepared by a facile freeze drying-assisted wet chemical route associated with a post-annealing process. When using as a cathode for lithium-ion battery (LIB), the designed LVP@NSC with N:S=1:2 exhibits outstanding high rate capacities of 124.4 and 107.85 mA h g-1 at 2 and 20 C in a voltage window of 3.0-4.3 V, respectively, and a ultralong cycle stability of 500 times at 20 C with remaining a reversible capacity of 100.22 mA h g−1 possibly due to its smallest charge transfer resistance and highest Li+ migration coefficiency, which is in good agreement with the theoretical rediction. This work not only reveals the critical role of interaction mechanism between NSC and LVP, but also offers great potentials for high energy density LIBs applications.