Kejian Li, Bingxing Zhang, Deming Xia, Zhengwei Ye, Yuyang Pan, Joseph S. Francisco, Zetian Mi
{"title":"Room-Temperature Catalyst-Free Ammonia Decomposition for Hydrogen Production on Water Microdroplets","authors":"Kejian Li, Bingxing Zhang, Deming Xia, Zhengwei Ye, Yuyang Pan, Joseph S. Francisco, Zetian Mi","doi":"10.1021/jacs.5c02072","DOIUrl":null,"url":null,"abstract":"Ammonia has been considered a viable carbon-free hydrogen carrier, yet its decomposition to hydrogen mainly relies on noble-metal-based catalysts and high temperatures. Here, through leveraging extraordinary physicochemical properties at the gas–liquid interface of water microdroplets, we present a catalyst-free and scalable approach for hydrogen production from ammonia under ambient conditions. A maximum hydrogen evolution rate of 226.8 μmol/h was observed, which outperformed most conventional catalytic methods at room temperature. Comprehensive experimental investigations and theoretical calculations revealed the underlying ammonia splitting mechanisms: hydroxyl radical and hydrogen radical, generated at the gas–liquid interface of microdroplets, synergistically triggered the interfacial ammonia decomposition following a thermodynamically favorable redox pathway, and the reaction rates can be enhanced by the high electric fields and reactants concentration accumulation at the gas–liquid interface. This work provides a new paradigm for green hydrogen production, advancing microdroplet chemistry and a sustainable hydrogen society.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"7 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2025-06-03","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.5c02072","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
Ammonia has been considered a viable carbon-free hydrogen carrier, yet its decomposition to hydrogen mainly relies on noble-metal-based catalysts and high temperatures. Here, through leveraging extraordinary physicochemical properties at the gas–liquid interface of water microdroplets, we present a catalyst-free and scalable approach for hydrogen production from ammonia under ambient conditions. A maximum hydrogen evolution rate of 226.8 μmol/h was observed, which outperformed most conventional catalytic methods at room temperature. Comprehensive experimental investigations and theoretical calculations revealed the underlying ammonia splitting mechanisms: hydroxyl radical and hydrogen radical, generated at the gas–liquid interface of microdroplets, synergistically triggered the interfacial ammonia decomposition following a thermodynamically favorable redox pathway, and the reaction rates can be enhanced by the high electric fields and reactants concentration accumulation at the gas–liquid interface. This work provides a new paradigm for green hydrogen production, advancing microdroplet chemistry and a sustainable hydrogen society.
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.