Noel J. Leon, Stefan Ilic, Xiaowei Xie, Heonjae Jeong, Zhenzhen Yang, Bingning Wang, Evan Walter Clark Spotte-Smith, Charlotte Stern, Nathan Hahn, Kevin Zavadil, Lei Cheng, Kristin A. Persson, Justin G. Connell and Chen Liao*,
{"title":"氧化铝钙电解质的设计原则和路线。","authors":"Noel J. Leon, Stefan Ilic, Xiaowei Xie, Heonjae Jeong, Zhenzhen Yang, Bingning Wang, Evan Walter Clark Spotte-Smith, Charlotte Stern, Nathan Hahn, Kevin Zavadil, Lei Cheng, Kristin A. Persson, Justin G. Connell and Chen Liao*, ","doi":"10.1021/acs.jpclett.4c00969","DOIUrl":null,"url":null,"abstract":"<p >Multivalent-ion battery technologies are increasingly attractive options for meeting diverse energy storage needs. Calcium ion batteries (CIB) are particularly appealing candidates for their earthly abundance, high theoretical volumetric energy density, and relative safety advantages. At present, only a few Ca-ion electrolyte systems are reported to reversibly plate at room temperature: for example, aluminates and borates, including Ca[TPFA]<sub>2</sub>, where [TPFA]<sup>−</sup> = [Al(OC(CF<sub>3</sub>)<sub>3</sub>)<sub>4</sub>]<sup>−</sup> and Ca[B(hfip)<sub>4</sub>]<sub>2</sub>, [B(hfip)<sub>4</sub>]<sub>2</sub><sup>–</sup> = [B(OCH(CF<sub>3</sub>)<sub>2</sub>)<sub>4</sub>]<sup>−</sup>. Analyzing the structure of these salts reveals a common theme: the prevalent use of a weakly coordinating anion (WCA) consisting of a tetracoordinate aluminum/boron (Al/B) center with fluorinated alkoxides. Leveraging the concept of theory-aided design, we report an innovative, one-pot synthesis of two new calcium-ion electrolyte salts (Ca[Al(tftb)<sub>4</sub>]<sub>2</sub>, Ca[Al(hftb)<sub>4</sub>]<sub>2</sub>) and two reported salts (Ca[Al(hfip)<sub>4</sub>]<sub>2</sub> and Ca[TPFA]<sub>2</sub>) where hfip = (−OCH(CF<sub>3</sub>)<sub>2</sub>), tftb = (−OC(CF<sub>3</sub>)(Me)<sub>2</sub>), hftb = (−OC(CF<sub>3</sub>)<sub>2</sub>(Me)), [TPFA]<sup>−</sup> = [Al(OC(CF<sub>3</sub>)<sub>3</sub>)<sub>4</sub>]<sup>−</sup>. We also reveal the dependence of Coulombic efficiency on their inherent propensity for cation–anion coordination.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 19","pages":"5096–5102"},"PeriodicalIF":4.6000,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Design Principles and Routes for Calcium Alkoxyaluminate Electrolytes\",\"authors\":\"Noel J. Leon, Stefan Ilic, Xiaowei Xie, Heonjae Jeong, Zhenzhen Yang, Bingning Wang, Evan Walter Clark Spotte-Smith, Charlotte Stern, Nathan Hahn, Kevin Zavadil, Lei Cheng, Kristin A. Persson, Justin G. Connell and Chen Liao*, \",\"doi\":\"10.1021/acs.jpclett.4c00969\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Multivalent-ion battery technologies are increasingly attractive options for meeting diverse energy storage needs. Calcium ion batteries (CIB) are particularly appealing candidates for their earthly abundance, high theoretical volumetric energy density, and relative safety advantages. At present, only a few Ca-ion electrolyte systems are reported to reversibly plate at room temperature: for example, aluminates and borates, including Ca[TPFA]<sub>2</sub>, where [TPFA]<sup>−</sup> = [Al(OC(CF<sub>3</sub>)<sub>3</sub>)<sub>4</sub>]<sup>−</sup> and Ca[B(hfip)<sub>4</sub>]<sub>2</sub>, [B(hfip)<sub>4</sub>]<sub>2</sub><sup>–</sup> = [B(OCH(CF<sub>3</sub>)<sub>2</sub>)<sub>4</sub>]<sup>−</sup>. Analyzing the structure of these salts reveals a common theme: the prevalent use of a weakly coordinating anion (WCA) consisting of a tetracoordinate aluminum/boron (Al/B) center with fluorinated alkoxides. Leveraging the concept of theory-aided design, we report an innovative, one-pot synthesis of two new calcium-ion electrolyte salts (Ca[Al(tftb)<sub>4</sub>]<sub>2</sub>, Ca[Al(hftb)<sub>4</sub>]<sub>2</sub>) and two reported salts (Ca[Al(hfip)<sub>4</sub>]<sub>2</sub> and Ca[TPFA]<sub>2</sub>) where hfip = (−OCH(CF<sub>3</sub>)<sub>2</sub>), tftb = (−OC(CF<sub>3</sub>)(Me)<sub>2</sub>), hftb = (−OC(CF<sub>3</sub>)<sub>2</sub>(Me)), [TPFA]<sup>−</sup> = [Al(OC(CF<sub>3</sub>)<sub>3</sub>)<sub>4</sub>]<sup>−</sup>. We also reveal the dependence of Coulombic efficiency on their inherent propensity for cation–anion coordination.</p>\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"15 19\",\"pages\":\"5096–5102\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2024-05-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpclett.4c00969\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpclett.4c00969","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Design Principles and Routes for Calcium Alkoxyaluminate Electrolytes
Multivalent-ion battery technologies are increasingly attractive options for meeting diverse energy storage needs. Calcium ion batteries (CIB) are particularly appealing candidates for their earthly abundance, high theoretical volumetric energy density, and relative safety advantages. At present, only a few Ca-ion electrolyte systems are reported to reversibly plate at room temperature: for example, aluminates and borates, including Ca[TPFA]2, where [TPFA]− = [Al(OC(CF3)3)4]− and Ca[B(hfip)4]2, [B(hfip)4]2– = [B(OCH(CF3)2)4]−. Analyzing the structure of these salts reveals a common theme: the prevalent use of a weakly coordinating anion (WCA) consisting of a tetracoordinate aluminum/boron (Al/B) center with fluorinated alkoxides. Leveraging the concept of theory-aided design, we report an innovative, one-pot synthesis of two new calcium-ion electrolyte salts (Ca[Al(tftb)4]2, Ca[Al(hftb)4]2) and two reported salts (Ca[Al(hfip)4]2 and Ca[TPFA]2) where hfip = (−OCH(CF3)2), tftb = (−OC(CF3)(Me)2), hftb = (−OC(CF3)2(Me)), [TPFA]− = [Al(OC(CF3)3)4]−. We also reveal the dependence of Coulombic efficiency on their inherent propensity for cation–anion coordination.
期刊介绍：
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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