Ultrafast sodium storage of alkylamine molecule tailored MnPS_(3) enabled by quasi-topological intercalation mechanism  

作　　者：Xueyang Tu Ke Fan Baixin Peng Zhuoran Lv Yiran Hao Wujie Dong Wei Zhao Zuocheng Wang Haitao Huang Yuqiang Fang Fuqiang Huang 

机构地区：[1]State Key Lab of Metal Matrix Composites,School of Materials Science and Engineering,Shanghai Jiao Tong University,Shanghai 200240,China [2]Zhangjiang Institute for Advanced Study,Shanghai Jiao Tong University,Shanghai 200240,China [3]State Key Laboratory of High-Performance Ceramics and Superfine Microstructure,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,China [4]Center of Materials Science and Optoelectronics Engineering,University of Chinese Academy of Sciences,Beijing 100049,China [5]Research Institute for Smart Energy,The Hong Kong Polytechnic University,Hong Kong 999077,China [6]Jiangxi Far East Battery Co.,Ltd.,Yichun 330600,China

出　　处：《Science China Chemistry》2025年第2期552-560,共9页中国科学(化学英文版)

基　　金：supported by the National Natural Science Foundation of China(52202327);the Science and Technology Commission of Shanghai Municipality(23DZ1200800,22ZR1471300);the China Postdoctoral Science Foundation(2023M742222,GZB20230400).

摘　　要：Two-dimensional transition metal trithiophosphates(TMPS_(3),TM=Mn,Fe,Co,etc.)are competitive anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity(>1,300 mAh g^(−1))but suffer from limited practical capacity(~300 mAh g^(−1))and inferior rate capability caused by sluggish Na+intercalation/deintercalation kinetics and severe structural collapse.Herein,alkylamine molecules are first proposed as intercalation guests to significantly boost the electrochemical activity and stability of MnPS_(3).Compared to MnPS_(3),C3H9N-MnPS_(3) enlarges the interlayer spacing from 6.48 to 10.23Åand shows a 105 times higher electrical conductivity,which provides fast ion/electron transport and high strain adaptability,realizing a quasi-topological Na+intercalation mechanism.Consequently,C3H9N-MnPS_(3) exhibits an ultrahigh reversible capacity of 775 mAh g^(−1) at 0.5 A g^(−1) and superior high-rate cycling stability with~100%capacity retention after 2,500 cycles at 15 A g^(−1),ranking it among the top metal trithiophosphate-based anode materials reported.Theoretical calculations indicate that the improved sodium storage performance of C3H9N-MnPS_(3) results from the reduced bonding energy of P–S bonds and increased adsorption energy of Na^(+).This work is expected to provide an efficient strategy for the design of high-performance layered anode materials for SIBs.

关 键 词：transition metal trithiophosphates intercalation guest sodium-ion batteries quasi-topological intercalation 

分 类 号：TM9[电气工程—电力电子与电力传动]