{"title":"铁心催化剂的配位工程,实现卓越的锂-S 电池性能。","authors":"Hao Yuan, Jing Yang, Yong-Wei Zhang","doi":"10.1002/asia.202400199","DOIUrl":null,"url":null,"abstract":"<p>Iron-nitrogen functionalized graphene has emerged as a promising cathode host for rechargeable lithium-sulfur batteries (RLSBs) due to its affordability and enhanced battery performance. To optimize its catalytical efficiency, we propose a novel approach involving coordination engineering. Our investigation spans a plethora of catalysts with varied coordination environments, focusing on elements B, C, N and O. We revealed that Fe−C<sub>4</sub> and Fe−B<sub>2</sub>C<sub>2</sub>−h are particularly effective for promoting Li<sub>2</sub>S oxidation, whereas Fe-N<sub>4</sub> excels in catalyzing the sulfur reduction reaction (SRR). Importantly, our study identified specific descriptors – namely, the Integrated Crystal Orbital Hamilton Population (ICOHP) and the bond length between Fe and S in Li<sub>2</sub>S adsorbed state – as the most effective predictive descriptors for Li<sub>2</sub>S oxidation barriers. Meanwhile, Li<sub>2</sub>S adsorption energy emerges as a reliable descriptor for assessing the SRR barrier. These identified descriptors are expected to be instrumental in rapidly identifying promising cathode hosts across various metal-centered systems with diverse coordination environments. Our findings not only offer valuable insights into the role of coordination environment, but also present an effective path for rapidly identifying high performance catalysts for RLSBs, enabling the acceleration of advanced RLSBs development.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":null,"pages":null},"PeriodicalIF":3.5000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Coordination Engineering of Fe-Centered Catalysts for Superior Li−S Battery Performance\",\"authors\":\"Hao Yuan, Jing Yang, Yong-Wei Zhang\",\"doi\":\"10.1002/asia.202400199\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Iron-nitrogen functionalized graphene has emerged as a promising cathode host for rechargeable lithium-sulfur batteries (RLSBs) due to its affordability and enhanced battery performance. To optimize its catalytical efficiency, we propose a novel approach involving coordination engineering. Our investigation spans a plethora of catalysts with varied coordination environments, focusing on elements B, C, N and O. We revealed that Fe−C<sub>4</sub> and Fe−B<sub>2</sub>C<sub>2</sub>−h are particularly effective for promoting Li<sub>2</sub>S oxidation, whereas Fe-N<sub>4</sub> excels in catalyzing the sulfur reduction reaction (SRR). Importantly, our study identified specific descriptors – namely, the Integrated Crystal Orbital Hamilton Population (ICOHP) and the bond length between Fe and S in Li<sub>2</sub>S adsorbed state – as the most effective predictive descriptors for Li<sub>2</sub>S oxidation barriers. Meanwhile, Li<sub>2</sub>S adsorption energy emerges as a reliable descriptor for assessing the SRR barrier. These identified descriptors are expected to be instrumental in rapidly identifying promising cathode hosts across various metal-centered systems with diverse coordination environments. Our findings not only offer valuable insights into the role of coordination environment, but also present an effective path for rapidly identifying high performance catalysts for RLSBs, enabling the acceleration of advanced RLSBs development.</p>\",\"PeriodicalId\":145,\"journal\":{\"name\":\"Chemistry - An Asian Journal\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2024-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemistry - An Asian Journal\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/asia.202400199\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry - An Asian Journal","FirstCategoryId":"1","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/asia.202400199","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Coordination Engineering of Fe-Centered Catalysts for Superior Li−S Battery Performance
Iron-nitrogen functionalized graphene has emerged as a promising cathode host for rechargeable lithium-sulfur batteries (RLSBs) due to its affordability and enhanced battery performance. To optimize its catalytical efficiency, we propose a novel approach involving coordination engineering. Our investigation spans a plethora of catalysts with varied coordination environments, focusing on elements B, C, N and O. We revealed that Fe−C4 and Fe−B2C2−h are particularly effective for promoting Li2S oxidation, whereas Fe-N4 excels in catalyzing the sulfur reduction reaction (SRR). Importantly, our study identified specific descriptors – namely, the Integrated Crystal Orbital Hamilton Population (ICOHP) and the bond length between Fe and S in Li2S adsorbed state – as the most effective predictive descriptors for Li2S oxidation barriers. Meanwhile, Li2S adsorption energy emerges as a reliable descriptor for assessing the SRR barrier. These identified descriptors are expected to be instrumental in rapidly identifying promising cathode hosts across various metal-centered systems with diverse coordination environments. Our findings not only offer valuable insights into the role of coordination environment, but also present an effective path for rapidly identifying high performance catalysts for RLSBs, enabling the acceleration of advanced RLSBs development.
期刊介绍:
Chemistry—An Asian Journal is an international high-impact journal for chemistry in its broadest sense. The journal covers all aspects of chemistry from biochemistry through organic and inorganic chemistry to physical chemistry, including interdisciplinary topics.
Chemistry—An Asian Journal publishes Full Papers, Communications, and Focus Reviews.
A professional editorial team headed by Dr. Theresa Kueckmann and an Editorial Board (headed by Professor Susumu Kitagawa) ensure the highest quality of the peer-review process, the contents and the production of the journal.
Chemistry—An Asian Journal is published on behalf of the Asian Chemical Editorial Society (ACES), an association of numerous Asian chemical societies, and supported by the Gesellschaft Deutscher Chemiker (GDCh, German Chemical Society), ChemPubSoc Europe, and the Federation of Asian Chemical Societies (FACS).