In situ Detection of the Molecule-Crowded Aqueous Electrode–Electrolyte Interface
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.
Authors
- Jiewu Cui (ORCID: https://orcid.org/0000-0003-4613-4795)
- Pengjun Zhang (ORCID: https://orcid.org/0000-0002-3104-1767)
- Xiaojun Wu (ORCID: https://orcid.org/0000-0003-3606-1211)
- Shiqiang Wei (ORCID: https://orcid.org/0000-0002-2052-1132)
- Yong Han (ORCID: https://orcid.org/0000-0002-9096-6516)
- Yixiu Wang (ORCID: https://orcid.org/0000-0002-4114-5113)
- Jialin Shi (ORCID: https://orcid.org/0000-0002-6853-619X)
- Zheng‐Hang Qi
- Hongwei Shou (ORCID: https://orcid.org/0000-0002-1012-5814)
- Shucheng Shi (ORCID: https://orcid.org/0000-0003-4568-9369)
- Shuangming Chen (ORCID: https://orcid.org/0000-0001-7567-1552)
- Li Song (ORCID: https://orcid.org/0000-0003-0585-8519)
- Zhi Liu (ORCID: https://orcid.org/0000-0002-8973-6561)
- Zijun Zhang (ORCID: https://orcid.org/0000-0002-2717-5033)
- Changda Wang (ORCID: https://orcid.org/0000-0002-3822-3475)
- Yuyang Cao
Institutions
- University of Science and Technology of China (CN)
- Hefei University of Technology (CN)
- Xinjiang Production and Construction Corps (CN)
- ShanghaiTech University (CN)
- Tarim University (CN)
- National Synchrotron Radiation Laboratory (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-03-19
- DOI
- https://doi.org/10.1021/jacs.4c14053
- Citations
- 11
- Primary Topic
- Advanced battery technologies research
- Type
- article
- Field-Weighted Citation Impact
- 8.03
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Youth Innovation Promotion Association of the Chinese Academy of Sciences
- Natural Science Foundation of Anhui Province
- National Key Research and Development Program of China
- Fundamental Research Funds for the Central Universities
- Anhui Provincial Key Research and Development Plan