Changjiang Hu, Junyi Zhao, Ruisi Chang, Hui Dong, Zhiwen Jiang, Xiang Li, Shinichi Yamashita, Pengfei Zheng, Degao Wang, Qing Huang, Xiaoping Ouyang, Yuxiang Bu, Shuao Wang, Jun Ma
{"title":"在环境条件下通过质子耦合的原位辐射分解电子转移从氮和水有效地生产氨","authors":"Changjiang Hu, Junyi Zhao, Ruisi Chang, Hui Dong, Zhiwen Jiang, Xiang Li, Shinichi Yamashita, Pengfei Zheng, Degao Wang, Qing Huang, Xiaoping Ouyang, Yuxiang Bu, Shuao Wang, Jun Ma","doi":"10.1021/jacs.5c11505","DOIUrl":null,"url":null,"abstract":"Ammonia (NH<sub>3</sub>) is a vital component for sustaining global food supplies and fuel production, but its industrial production via the Haber–Bosch process remains energetically demanding and carbon-intensive. Here, we report an electron-beam-activated NH<sub>3</sub> synthesis strategy that utilizes only atmospheric N<sub>2</sub> and water as feedstocks under ambient conditions. This approach achieves an industrially relevant rate of 83.6 μmol g<sup>–1</sup> s<sup>–1</sup> with a substantially improved energy efficiency of 0.53 MJ/mol, which surpasses most laboratory-scale technologies and is comparable to that of the Haber–Bosch process. Time-resolved operando spectroscopic experiments, combined with theoretical calculations, reveal that this distinct activation mode enables rapid N<sub>2</sub>→NH<sub>3</sub> conversion through a proton-coupled transfer of an in situ generated energetic hydrated electron. Furthermore, techno-economic analysis and life-cycle assessment demonstrate that the operational simplicity and exceptional throughput of the present N<sub>2</sub> fixation approach could promote nitrogen circularity in the sustainable chemical industry.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"11 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effective Ammonia Production from Nitrogen and Water under Ambient Conditions through Proton-Coupled In Situ Radiolytic Electron Transfer\",\"authors\":\"Changjiang Hu, Junyi Zhao, Ruisi Chang, Hui Dong, Zhiwen Jiang, Xiang Li, Shinichi Yamashita, Pengfei Zheng, Degao Wang, Qing Huang, Xiaoping Ouyang, Yuxiang Bu, Shuao Wang, Jun Ma\",\"doi\":\"10.1021/jacs.5c11505\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Ammonia (NH<sub>3</sub>) is a vital component for sustaining global food supplies and fuel production, but its industrial production via the Haber–Bosch process remains energetically demanding and carbon-intensive. Here, we report an electron-beam-activated NH<sub>3</sub> synthesis strategy that utilizes only atmospheric N<sub>2</sub> and water as feedstocks under ambient conditions. This approach achieves an industrially relevant rate of 83.6 μmol g<sup>–1</sup> s<sup>–1</sup> with a substantially improved energy efficiency of 0.53 MJ/mol, which surpasses most laboratory-scale technologies and is comparable to that of the Haber–Bosch process. Time-resolved operando spectroscopic experiments, combined with theoretical calculations, reveal that this distinct activation mode enables rapid N<sub>2</sub>→NH<sub>3</sub> conversion through a proton-coupled transfer of an in situ generated energetic hydrated electron. Furthermore, techno-economic analysis and life-cycle assessment demonstrate that the operational simplicity and exceptional throughput of the present N<sub>2</sub> fixation approach could promote nitrogen circularity in the sustainable chemical industry.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"11 1\",\"pages\":\"\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-10-02\",\"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.5c11505\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.5c11505","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Effective Ammonia Production from Nitrogen and Water under Ambient Conditions through Proton-Coupled In Situ Radiolytic Electron Transfer
Ammonia (NH3) is a vital component for sustaining global food supplies and fuel production, but its industrial production via the Haber–Bosch process remains energetically demanding and carbon-intensive. Here, we report an electron-beam-activated NH3 synthesis strategy that utilizes only atmospheric N2 and water as feedstocks under ambient conditions. This approach achieves an industrially relevant rate of 83.6 μmol g–1 s–1 with a substantially improved energy efficiency of 0.53 MJ/mol, which surpasses most laboratory-scale technologies and is comparable to that of the Haber–Bosch process. Time-resolved operando spectroscopic experiments, combined with theoretical calculations, reveal that this distinct activation mode enables rapid N2→NH3 conversion through a proton-coupled transfer of an in situ generated energetic hydrated electron. Furthermore, techno-economic analysis and life-cycle assessment demonstrate that the operational simplicity and exceptional throughput of the present N2 fixation approach could promote nitrogen circularity in the sustainable chemical industry.
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.