High-energy silicon-sulfurized poly(acrylonitrile)battery based on a nitrogen evolution reaction  

一种基于析氮反应的新型高比能硅-硫化聚(丙烯腈)电池

作　　者：Pengfei Wang Chao Xia Jingui Yang Xuewei He Kezhong Lv Siyun Ren Hucheng Song Jiulin Wang Ping He Haoshen Zhou 王鹏飞;夏潮;杨金贵;何学威;吕可中;任思赞;宋虎成;王久林;何平;周豪慎(Center of Energy Storage Materials&Technology,College of Engineering and Applied Sciences,Jiangsu Key Laboratory of Artificial Functional Materials,National Laboratory of Solid State Microstructures,and Collaborative Innovation Center of Advanced Microstructures,Nanjing University,Nanjing 210023,China;Shanghai Electrochemical Energy Devices Research Center,School of Chemistry and Chemical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China)

机构地区：[1]Center of Energy Storage Materials&Technology,College of Engineering and Applied Sciences,Jiangsu Key Laboratory of Artificial Functional Materials,National Laboratory of Solid State Microstructures,and Collaborative Innovation Center of Advanced Microstructures,Nanjing University,Nanjing 210023,China [2]Shanghai Electrochemical Energy Devices Research Center,School of Chemistry and Chemical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China

出　　处：《Science Bulletin》2022年第3期256-262,共7页科学通报（英文版）

基　　金：the National Natural Science Foundation of China(21922508,21673116,21633003,and U1801251);Natural Science Foundation of Jiangsu Province of China(BK20190009);and Key R&D Project funded by Department of Science and Technology of Jiangsu Province(BE2020003)。

摘　　要：The practical application of high-energy lithium–sulfur battery is plagued with two deadly obstacles.One is the“shuttle effect”originated from the sulfur cathode,and the other is the low Coulombic efficiency and security issues arising from the lithium metal anode.In addressing these issues,we propose a novel silicon-sulfurized poly(acrylonitrile)full battery.In this lithium metal-free system,the Li source is pre-loaded in the cathode,using a nitrogen evolution reaction(NER)to implant Li+into the silicon/carbon anode.Sulfurized poly(acrylonitrile)based on a solid–solid conversion mechanism can fundamentally circumvent the“shuttle effect”.Meanwhile,the silicon/carbon anode can achieve more efficient utiliza-tion and higher security when compared with the Li metal anode.The full cell used in this technology can deliver a capacity of 1169.3 mAh g^(-1),and it can be stabilized over 100 cycles,implying its excellent elec-trochemical stability.Furthermore,the practical pouch cell with a high sulfur loading of 4.2 mg cm^(-2)can achieve a high specific energy of 513.2 Wh kg-1.The mechanism of the NER in cathode has also been investigated and analyzed by in situ methods.Notably,this battery design completely conforms to the current battery production technology because of the degassing of gasbag,resulting in a low manufactur-ing cost.This work will open the avenue to develop a lithium metal-free battery using the NER.高比能锂-硫电池的实际应用面临两大致命障碍:一是源于硫正极的“穿梭效应”,二是锂金属负极带来的低库仑效率和安全问题,为了彻底解决这些问题,本文提出了一种新型的硅-硫化聚(丙烯腈)全电池。在这种不含锂金属的系统中,锂源被预加载在正极中,采用析氮反应将锂离子注入硅基负极.基于固-固转化机制的硫化聚(丙烯腈)正极可以从根本上规避“穿梭效应”.同时,与锂金属负极相比,硅基负极可以实现更有效的利用和更高的安全性.采用该技术的全电池可提供1169.3mAhg^(-1)的容量并稳定循环100次,显示出优异的电化学稳定性.此外,即使在4.2 mgcm^(-2)高硫载量的实用软包电池也可以实现513.2 Whkg^(-1)的高比能量.本文还通过原位方法研究和分析了正极中析氮反应的机制.值得注意的是,这种电池设计完全匹配当前的电池生产工艺,制造成本低,为采用析氨反应开发无金属锂电池开辟道路.

关 键 词：Nitrogen evolution reaction High specific energy Silicon-sulfur battery Lithium metal-free High Coulombic efficiency 

分 类 号：O646[理学—物理化学] TM912[理学—化学]