Synergistic Redox Dual-Site Strategy to Boost Photosynthesis of Hydrogen Peroxide

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Rongao Zhang, Haonan Xu, Zixiang Huang, Jing Zhang, Limin Liu, Zhentao Ma, Zhilin Zhang, Kun Wang, Peigen Liu, Huarong Liu, Xusheng Zheng
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Abstract

Graphitized carbon nitride (C3N4)-based photocatalysts provide a prospective approach for producing hydrogen peroxide (H2O2) in artificial photosynthesis. However, their activity is constrained by the sluggish water oxidation reaction (WOR) process, which hampers the supply of protons and electrons necessary for the oxygen reduction reaction. Here, this work demonstrates a synergistic redox dual-site strategy via co-modified with 3,4,9,10-perylenetetracarboxylic acid diimide (PDI) and Pt single atoms in C3N4 support, which achieves an exceptional H2O2 yield of 802 µmol g−1 h−1 and a selectivity of 91.8% without sacrificial agents. Mechanistic studies reveal that Pt single atoms act as photogenerated electron-rich sites to effectively activate O2 to form superoxide radicals, and PDI promotes WOR driving force to provide abundant protons. The optimized reduction and oxidation half-reactions improve the proton-coupled electron transfer process, thereby enhancing the selective photosynthesis of H2O2. This work underscores the importance of finely controlling half-reactions in photocatalytic processes to promote efficient and synergistic overall reactions.

Abstract Image

协同氧化还原双位点策略促进过氧化氢的光合作用
石墨化氮化碳(C3N4)基光催化剂为人工光合作用生成过氧化氢(H2O2)提供了一种有前景的途径。然而,它们的活性受到缓慢的水氧化反应(WOR)过程的限制,这阻碍了氧还原反应所需的质子和电子的供应。本研究通过在C3N4载体上对3,4,9,10-苝四羧酸二亚胺(PDI)和Pt单原子进行共修饰,证明了一种协同氧化还原双位点策略,该策略在没有牺牲剂的情况下获得了802µmol g−1 h−1的H2O2产率和91.8%的选择性。机理研究表明,Pt单原子作为光生富电子位点有效激活O2形成超氧自由基,PDI促进WOR驱动力提供丰富的质子。优化后的还原和氧化半反应改善了质子耦合电子传递过程,从而增强了H2O2的选择性光合作用。这项工作强调了在光催化过程中精细控制半反应以促进高效和协同的整体反应的重要性。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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