文献类型：期刊文献

英文题名：Dual-Quenching Charge Transfer Unlocks Record Nitrate-to-Ammonia Photocatalytic Conversion in Redox-Active Eosin Y Polymers

作者：Zhang, Jiayi[1,2];Chen, Dingming[1,2];Tian, Limei[3,4];Feng, Shufan[1,2,5,6,7];Li, Zihan[1,2];Yu, Zhiwu[1,2];Zhou, Min[1,2];Wang, Haifeng[1,2];Hu, Ke[3,4,8];Hua, Jianli[1,2]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Joint Int Res Lab Precis Chem, Shanghai, Peoples R China;[3]Fudan Univ, Dept Chem, Shanghai, Peoples R China;[4]Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai, Peoples R China;[5]Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Hangzhou, Peoples R China;[6]Westlake Univ, Sch Sci, Dept Chem, Hangzhou, Peoples R China;[7]Westlake Univ, Res Ctr Ind Future, Hangzhou, Peoples R China;[8]Tongji Univ, Sch Chem Sci & Engn, Shanghai, Peoples R China

年份：2026

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20262420904712);WOS:【SCI-EXPANDED(收录号:WOS:001791112900001)】；

基金：For financial support of this research, the authors thank the projects supported by the National Natural Science Foundation of China (22271093, 21971064, and 22173022), the Science and Technology Commission of Shanghai Municipality (24DX1400200), the Programme of Introducing Talents of Discipline to Universities (B16017), the Fundamental Research Funds for the Central Universities. The authors thank the Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：ammonia; Eosin Y; ground-state complexation; photocatalytic nitrate reduction; radical intermediates

摘要：Efficient photocatalytic nitrate reduction reaction (NO3RR) is vital for mitigating nitrogen pollution and producing green ammonia (NH3). Although organic polymer photocatalysts show great potential for NO3RR, they frequently suffer from low charge separation efficiency. This limitation largely comes from the lack of suitable redox-active moieties incorporated in the polymer photocatalysts toward NO3RR. Herein, we embed the redox-active Eosin Y (EY) into a conjugated polymer backbone to synthesize a series of EY-X polymers (where X = benzene, biphenyl, or fluorene), in which the extended pi-conjugation can promote dual dynamic and static quenching for directional electron transfer. Upon visible-light excitation, EY forms a long-lived radical anion (EY center dot-) that stores and relays electrons to nitrate, while ground-state complexation between polymer and nitrate preorganizes the substrate for photoinduced directional electron transfer. This dual-pathway mechanism extends charge-separated lifetimes, inhibits recombination, and enhances electron delivery. Consequently, under cocatalyst-free conditions, the EY-BE polymer achieves a record high NH3 production of 215 & micro;mol g-1 h-1. Experimental and computational investigations support the reversible EY/EY center dot- cycle and the nitrate-binding ground-state complex as the origin of activity and selectivity. This work demonstrates a rational strategy leveraging reversible redox-active chromophores to integrate dual quenching for designing high-performance NO3RR photocatalysts.