文献类型：期刊文献

英文题名：Proton-Enriched Alginate-Graphene Hydrogel Microreactor for Enhanced Hydrogen Peroxide Photosynthesis

作者：He, Chun[1,2];Lei, Juying[3];Li, Xiang[1,2];Shen, Ziyun[1,2];Wang, Lingzhi[1,2];Zhang, Jinlong[1,2]

机构：[1]East China Univ, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Key Lab Adv Mat,Joint Int Res Lab Precis Chem & Mo, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Natl Engn Res Ctr Ind Wastewater Detoxicat & Resou, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China

年份：2024

卷号：63

期号：40

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20243616996169);WOS:【SCI-EXPANDED(收录号:WOS:001302738200001)】；

基金：This work was supported by National Key R&D Program of China (2022YFE0107900), National Natural Science Foundation of China (21822603 and 21773062), Shanghai Municipal Science and Technology Major Project (2018SHZDZX03), the Science and Technology Commission of Shanghai Municipality (21ZR1417900, 17520711500, 22230780200, and 20DZ2250400), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), and the Fundamental Research Funds for the Central Universities (222201717003).

语种：英文

外文关键词：Photocatalysis; Gels; Hydrogen Peroxide; Oxygen Reduction Reaction

摘要：Efficient synthesis of H2O2 via photocatalytic oxygen reduction without sacrificial agents is challenging due to inadequate proton supply from water and difficulty in maintaining O-O bond during O2 activation. Herein, we developed a straightforward strategy involving a proton-rich hydrogel cross-linked by metal ions [M(n)], which is designed to facilitate the selective production of H2O2 through proton relay and metal ion-assisted detachment of crucial intermediates. The hydrogel comprises CdS/graphene and alginate cross-linked by metal ions via O=C-O-M(n) bonds. Efficient O2 reduction and hydrogenation occurred, benefitting from the collaboration between proton-rich alginate and the photocatalytically active CdS/graphene. Meanwhile, the O=C-O-M(n) bonds enhance the electron density of alpha-carbon sites on graphene, crucial for O2 activation and *OOH intermediate detachment, preventing deeper O-O bond cleavage. The role of metal ions in promoting *OOH desorption was demonstrated through Lewis acidity-dependent activity, with Y(III) having the highest activity, followed by Lu(III), La(III), and Ca(II). This study establishes a graphene-alginate hydrogel system cross-linked by metal ions M(n), addressing the challenges of insufficient proton supply and stable detachment of the intermediate *OOH in photocatalytic ORR reactions. The alginate framework facilitates proton relay, while the role of metal ions was evident through Lewis acidity-dependent activity for H2O2 production. image