Yimei Chen, Kaijie Zhang, Zhixiao Xu, Facheng Gong, Renfei Feng, Zhehui Jin and Xiaolei Wang
{"title":"通过电解质化学调节界面反应,为宽温锌金属电池提供富含阴离子的间相","authors":"Yimei Chen, Kaijie Zhang, Zhixiao Xu, Facheng Gong, Renfei Feng, Zhehui Jin and Xiaolei Wang","doi":"10.1039/D4EE04803B","DOIUrl":null,"url":null,"abstract":"<p >Zinc-ion batteries are challenged by zinc dendrites, notorious side reactions, and poor performance at low temperatures. Here, we present a dual-salt tuned electrolyte exhibiting a wide temperature range (−60 to 25 °C). The Zn(ClO<small><sub>4</sub></small>)<small><sub>2</sub></small>-based electrolyte with high hydrogen bond destruction ability and fast diffusion kinetics is suitable for application at ultralow temperatures. The introduction of Zn(OAc)<small><sub>2</sub></small> salt enhances cation–anion interaction and facilitates the formation of an anion-rich solvation shell and salt-derived interphase, overcoming issues caused by the strong oxidation of ClO<small><sub>4</sub></small><small><sup>−</sup></small> in the presence of protons. The selective absorption of OAc<small><sup>−</sup></small> on different zinc crystal planes favors dense zinc deposition towards (101) epitaxial while the as-formed anion-rich SEI layer, featuring 2ZnCO<small><sub>3</sub></small>·3Zn(OH)<small><sub>2</sub></small> distributed on the surface and ZnCl<small><sub>2</sub></small> uniformly dispersed throughout, inhibits side reactions of corrosion and hydrogen evolution. Consequently, the batteries employing the designed electrolyte exhibited excellent performances, including a high Coulombic efficiency of 99.5% over 800 cycles at 25 °C; a near-unity Coulombic efficiency (100%) for over 4000 cycles and long cycling stability for over 5 months (16 500 cycles) in a Zn//I<small><sub>2</sub></small> battery with an accumulative capacity of 7300 mA h cm<small><sup>−2</sup></small> at −40 °C. Even at −60 °C, the solid-state electrolyte demonstrates practical applicability in Zn‖I<small><sub>2</sub></small>/AC and Zn‖VO<small><sub>2</sub></small> batteries. This dual salt-tuned pure aqueous electrolyte also allows the reversible operation of a pouch cell for over 10 000 cycles with an accumulative capacity of 19.0 A h, indicating its promising potential for constructing safe and environmentally friendly zinc-ion batteries with broad working temperatures.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 713-727"},"PeriodicalIF":32.4000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Regulating interfacial reactions through electrolyte chemistry enables an anion-rich interphase for wide-temperature zinc metal batteries†\",\"authors\":\"Yimei Chen, Kaijie Zhang, Zhixiao Xu, Facheng Gong, Renfei Feng, Zhehui Jin and Xiaolei Wang\",\"doi\":\"10.1039/D4EE04803B\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Zinc-ion batteries are challenged by zinc dendrites, notorious side reactions, and poor performance at low temperatures. Here, we present a dual-salt tuned electrolyte exhibiting a wide temperature range (−60 to 25 °C). The Zn(ClO<small><sub>4</sub></small>)<small><sub>2</sub></small>-based electrolyte with high hydrogen bond destruction ability and fast diffusion kinetics is suitable for application at ultralow temperatures. The introduction of Zn(OAc)<small><sub>2</sub></small> salt enhances cation–anion interaction and facilitates the formation of an anion-rich solvation shell and salt-derived interphase, overcoming issues caused by the strong oxidation of ClO<small><sub>4</sub></small><small><sup>−</sup></small> in the presence of protons. The selective absorption of OAc<small><sup>−</sup></small> on different zinc crystal planes favors dense zinc deposition towards (101) epitaxial while the as-formed anion-rich SEI layer, featuring 2ZnCO<small><sub>3</sub></small>·3Zn(OH)<small><sub>2</sub></small> distributed on the surface and ZnCl<small><sub>2</sub></small> uniformly dispersed throughout, inhibits side reactions of corrosion and hydrogen evolution. Consequently, the batteries employing the designed electrolyte exhibited excellent performances, including a high Coulombic efficiency of 99.5% over 800 cycles at 25 °C; a near-unity Coulombic efficiency (100%) for over 4000 cycles and long cycling stability for over 5 months (16 500 cycles) in a Zn//I<small><sub>2</sub></small> battery with an accumulative capacity of 7300 mA h cm<small><sup>−2</sup></small> at −40 °C. Even at −60 °C, the solid-state electrolyte demonstrates practical applicability in Zn‖I<small><sub>2</sub></small>/AC and Zn‖VO<small><sub>2</sub></small> batteries. This dual salt-tuned pure aqueous electrolyte also allows the reversible operation of a pouch cell for over 10 000 cycles with an accumulative capacity of 19.0 A h, indicating its promising potential for constructing safe and environmentally friendly zinc-ion batteries with broad working temperatures.</p>\",\"PeriodicalId\":72,\"journal\":{\"name\":\"Energy & Environmental Science\",\"volume\":\" 2\",\"pages\":\" 713-727\"},\"PeriodicalIF\":32.4000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Environmental Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2025/ee/d4ee04803b\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Environmental Science","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/ee/d4ee04803b","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Regulating interfacial reactions through electrolyte chemistry enables an anion-rich interphase for wide-temperature zinc metal batteries†
Zinc-ion batteries are challenged by zinc dendrites, notorious side reactions, and poor performance at low temperatures. Here, we present a dual-salt tuned electrolyte exhibiting a wide temperature range (−60 to 25 °C). The Zn(ClO4)2-based electrolyte with high hydrogen bond destruction ability and fast diffusion kinetics is suitable for application at ultralow temperatures. The introduction of Zn(OAc)2 salt enhances cation–anion interaction and facilitates the formation of an anion-rich solvation shell and salt-derived interphase, overcoming issues caused by the strong oxidation of ClO4− in the presence of protons. The selective absorption of OAc− on different zinc crystal planes favors dense zinc deposition towards (101) epitaxial while the as-formed anion-rich SEI layer, featuring 2ZnCO3·3Zn(OH)2 distributed on the surface and ZnCl2 uniformly dispersed throughout, inhibits side reactions of corrosion and hydrogen evolution. Consequently, the batteries employing the designed electrolyte exhibited excellent performances, including a high Coulombic efficiency of 99.5% over 800 cycles at 25 °C; a near-unity Coulombic efficiency (100%) for over 4000 cycles and long cycling stability for over 5 months (16 500 cycles) in a Zn//I2 battery with an accumulative capacity of 7300 mA h cm−2 at −40 °C. Even at −60 °C, the solid-state electrolyte demonstrates practical applicability in Zn‖I2/AC and Zn‖VO2 batteries. This dual salt-tuned pure aqueous electrolyte also allows the reversible operation of a pouch cell for over 10 000 cycles with an accumulative capacity of 19.0 A h, indicating its promising potential for constructing safe and environmentally friendly zinc-ion batteries with broad working temperatures.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).