Wu Zelin, Wu Yunjia, Yuan Qingyan, Zhang Jian, Dou Yibo, Han Jingbin
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China.
Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, Zhejiang, P. R. China.
ACS Appl Mater Interfaces. 2023 Aug 16;15(32):38540-38549. doi: 10.1021/acsami.3c09706. Epub 2023 Aug 7.
Aqueous chloride-ion batteries (ACIBs) with environmental friendliness and high safety hold great potential to fulfill the green energy demand for ocean desalination. Herein, for the first time, a composite consisting of Cl-intercalated CoFe layered double hydroxides (CoFe-Cl-LDH) cross-linked with CNTs (CoFe-Cl-LDH/CNT) is synthesized and demonstrated to be a novel high-performance anode for ACIBs in a neutral NaCl aqueous solution. While exhibiting a high initial capacity of ∼190 mAh g at 200 mA g, CoFe-Cl-LDH/CNT is capable of delivering a reversible capacity of ∼125 mAh g after 200 cycles. At a high current density of 400 mA g, it still holds a capacity of ∼120 mAh g. The excellent Cl storage performance can be contributed to the unique topochemical transformation feature that reverses intercalation/deintercalation of Cl along with valence changes of Co/Co and Fe/Fe during charge/discharge and the improved electronic conductivity by hybridizing with CNTs. It is interesting that the invertible insertion/extraction of interlayer HO was discovered, which could be beneficial to the capacity after cycles to a certain extent. The Cl-intercalated LDH material declared in this work shows its feasibility on Cl capture/release in aqueous anion-type batteries and provides a new opportunity for future development of ACIBs or aqueous desalination technology.
具有环境友好性和高安全性的水系氯离子电池（ACIBs）在满足海洋淡化的绿色能源需求方面具有巨大潜力。在此，首次合成了一种由与碳纳米管（CNT）交联的Cl插层CoFe层状双氢氧化物（CoFe-Cl-LDH）组成的复合材料，并证明其在中性NaCl水溶液中是一种新型的高性能ACIBs阳极。CoFe-Cl-LDH/CNT在200 mA g下表现出约190 mAh g的高初始容量，在200次循环后能够提供约125 mAh g的可逆容量。在400 mA g的高电流密度下，它仍保持约120 mAh g的容量。优异的Cl存储性能可归因于独特的拓扑化学转变特性，即在充放电过程中，Cl的嵌入/脱嵌与Co/Co和Fe/Fe的价态变化同时发生逆转，以及通过与CNT杂化提高了电子导电性。有趣的是，发现了层间HO的可逆插入/提取，这在一定程度上可能有利于循环后的容量。本文报道的Cl插层LDH材料展示了其在水系阴离子型电池中Cl捕获/释放的可行性，并为ACIBs或水系淡化技术的未来发展提供了新的机遇。
