{"title":"Optimizing the p charge of S in p-block metal sulfides for sulfur reduction electrocatalysis","authors":"Wuxing Hua, Tongxin Shang, Huan Li, Yafei Sun, Yong Guo, Jingyi Xia, Chuannan Geng, Zhonghao Hu, Linkai Peng, Zhiyuan Han, Chen Zhang, Wei Lv, Ying Wan","doi":"10.1038/s41929-023-00912-9","DOIUrl":null,"url":null,"abstract":"Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p-block metal sulfides and the apparent activation energies (Ea) for the sulfur reduction reaction (SRR), in particular, Li2Sn to Li2S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest Ea and a high SRR rate in the cathode. Li–S batteries with the Bi2S3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm−2 was obtained under a high sulfur loading of 17.6 mg cm−2 but a low electrolyte/sulfur ratio of 7.5 μl mg−1. Lithium–sulfur batteries are promising energy storage devices where catalysis can play an important role, but developing design principles for optimal performance remains a challenge. Now, a series of p-block metal sulfide cathodes are evaluated, revealing a direct correlation between the p electron gain of sulfur in the sulfide material and the apparent activation energy for the sulfur reduction reaction.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8000,"publicationDate":"2023-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"13","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.nature.com/articles/s41929-023-00912-9","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 13
Abstract
Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p-block metal sulfides and the apparent activation energies (Ea) for the sulfur reduction reaction (SRR), in particular, Li2Sn to Li2S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest Ea and a high SRR rate in the cathode. Li–S batteries with the Bi2S3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm−2 was obtained under a high sulfur loading of 17.6 mg cm−2 but a low electrolyte/sulfur ratio of 7.5 μl mg−1. Lithium–sulfur batteries are promising energy storage devices where catalysis can play an important role, but developing design principles for optimal performance remains a challenge. Now, a series of p-block metal sulfide cathodes are evaluated, revealing a direct correlation between the p electron gain of sulfur in the sulfide material and the apparent activation energy for the sulfur reduction reaction.
期刊介绍:
Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry.
Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.