{"title":"Steering artificial photosynthesis via photoinduced conversion of monometallic to bimetallic sites in FeCo nitroprussides.","authors":"Hao Wang, Gui-Lin Zhuang, Yingjie Fan, Hua-Qing Yin, Wei Zhang, Zhe Wu, Shuang Yao, Tong-Bu Lu, Wenbin Lin, Zhi-Ming Zhang","doi":"10.1038/s41467-025-61129-x","DOIUrl":null,"url":null,"abstract":"<p><p>Artificial photosynthesis provides an efficient strategy for solar energy storage via water splitting and CO<sub>2</sub> reduction, but it remains a challenge in tuning artificial photosynthesis between these two competing reactions. Herein, we demonstrate photoinduced conversion of monometallic to bimetallic sites in a Fe-Co nitroprusside (FeCo-NP) to steer the reaction path from H<sub>2</sub> evolution to CO<sub>2</sub> reduction. Monometallic Co sites achieve efficient H<sub>2</sub> production with 28.5 mmol g<sup>-1</sup> activity and 85.4% selectivity. Photoinduced release of nitrosyl groups from Fe sites generates bimetallic Fe-Co sites, which suppress H<sub>2</sub> evolution and enhance CO<sub>2</sub> reduction, yielding 31.5 mmol g<sup>-1</sup> activity and 87.3% selectivity for C1 products. Mechanistic investigations reveal that monometallic Co sites catalyze H<sub>2</sub> evolution via H<sub>2</sub>O adsorption and O-H cleavage while bimetallic Fe-Co sites facilitate both H<sub>2</sub>O and CO<sub>2</sub> adsorption and subsequent O and C hydrogenation for CO and HCOOH. This work uncovers a strategy to manipulate competing reaction pathways via photoinduced conversion of monometallic to bimetallic sites, which provides unique insights into addressing environmental issues and energy crises.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"16 1","pages":"6160"},"PeriodicalIF":14.7000,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-61129-x","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
Artificial photosynthesis provides an efficient strategy for solar energy storage via water splitting and CO2 reduction, but it remains a challenge in tuning artificial photosynthesis between these two competing reactions. Herein, we demonstrate photoinduced conversion of monometallic to bimetallic sites in a Fe-Co nitroprusside (FeCo-NP) to steer the reaction path from H2 evolution to CO2 reduction. Monometallic Co sites achieve efficient H2 production with 28.5 mmol g-1 activity and 85.4% selectivity. Photoinduced release of nitrosyl groups from Fe sites generates bimetallic Fe-Co sites, which suppress H2 evolution and enhance CO2 reduction, yielding 31.5 mmol g-1 activity and 87.3% selectivity for C1 products. Mechanistic investigations reveal that monometallic Co sites catalyze H2 evolution via H2O adsorption and O-H cleavage while bimetallic Fe-Co sites facilitate both H2O and CO2 adsorption and subsequent O and C hydrogenation for CO and HCOOH. This work uncovers a strategy to manipulate competing reaction pathways via photoinduced conversion of monometallic to bimetallic sites, which provides unique insights into addressing environmental issues and energy crises.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.