{"title":"In situ Detection of the Molecule-Crowded Aqueous Electrode–Electrolyte Interface","authors":"Shiqiang Wei, Hongwei Shou, Zheng-Hang Qi, Shuangming Chen, Yong Han, Shucheng Shi, Yixiu Wang, Pengjun Zhang, Jialin Shi, Zijun Zhang, Yuyang Cao, Changda Wang, Jiewu Cui, Xiaojun Wu, Zhi Liu, Li Song","doi":"10.1021/jacs.4c14053","DOIUrl":null,"url":null,"abstract":"Electrode–electrolyte interface plays a crucial role in determining the stability and behavior of electrochemical electrodes. Although X-ray photoelectron spectroscopy has been established as a powerful analytical technique for interface chemistry, the necessity for ultrahigh vacuum remains a significant obstacle to directly detecting dynamic interfacial evolution, particularly in aqueous environments. Here, we employ tender-energy ambient pressure X-ray photoelectron spectroscopy (AP-XPS) to bridge the gap between ultrahigh vacuum and near-atmospheric pressure, enabling an in-depth investigation of the molecule-crowded aqueous interface evolution in a Zn metal anode. The results demonstrate that the persistent presence of additive molecules effectively inhibits direct contact between reactive Zn and H<sub>2</sub>O, while also facilitating uniform Zn deposition. In situ optical microscopy observations and synchrotron radiation X-ray diffraction further verified the uniform and dense Zn deposition, attributed to lateral growth induced by the (002) crystal facet evolution. As proof of its effectiveness, batteries incorporating the Zn//Zn, Zn//Cu, and full cell with the additive demonstrate significantly improved stability and reversibility. This finding opens up new avenues for exploration of interfacial chemistry at the molecule level, offering insights into the design of highly stable metal anodes of aqueous ion batteries for practical applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"7 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c14053","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Electrode–electrolyte interface plays a crucial role in determining the stability and behavior of electrochemical electrodes. Although X-ray photoelectron spectroscopy has been established as a powerful analytical technique for interface chemistry, the necessity for ultrahigh vacuum remains a significant obstacle to directly detecting dynamic interfacial evolution, particularly in aqueous environments. Here, we employ tender-energy ambient pressure X-ray photoelectron spectroscopy (AP-XPS) to bridge the gap between ultrahigh vacuum and near-atmospheric pressure, enabling an in-depth investigation of the molecule-crowded aqueous interface evolution in a Zn metal anode. The results demonstrate that the persistent presence of additive molecules effectively inhibits direct contact between reactive Zn and H2O, while also facilitating uniform Zn deposition. In situ optical microscopy observations and synchrotron radiation X-ray diffraction further verified the uniform and dense Zn deposition, attributed to lateral growth induced by the (002) crystal facet evolution. As proof of its effectiveness, batteries incorporating the Zn//Zn, Zn//Cu, and full cell with the additive demonstrate significantly improved stability and reversibility. This finding opens up new avenues for exploration of interfacial chemistry at the molecule level, offering insights into the design of highly stable metal anodes of aqueous ion batteries for practical applications.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.