文献类型：期刊文献

英文题名：Molecular Assembly Unlocks Dual-Defect Synergy in Carbon Nitride for Efficient H2O2 Photosynthesis

作者：Sun, Xiaolin[1];Tian, Pengfei[2];Li, Jinye[1];Zhu, Minghui[1];Xu, Jing[1,3];Xuan, Fu-Zhen[2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Mech & Power Engn, Key Lab Pressure Syst & Safety, Minist Educ, Shanghai 200237, Peoples R China;[3]Guangxi Univ, Univ Engn Res Ctr Green Chem New Mat, Sch Chem & Chem Engn, Nanning 530004, Guangxi, Peoples R China

年份：2026

卷号：13

期号：5

外文期刊名：ADVANCED SCIENCE

收录：;EI(收录号：20254619498236);WOS:【SCI-EXPANDED(收录号:WOS:001610083000001)】；

基金：This work was supported by the National Natural Science Foundation of China (22521201, 22578125). Shanghai Pilot Program for Basic Research (22TQ1400100-7), the Basic Research Program of Science and Technology Commission of Shanghai Municipality (22JC1400600) and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：defected carbon nitride; hydrogen peroxide synthesis; molecular assembly-molten salt coupling; Photocatalytic oxygen reduction

摘要：While promising for photocatalytic hydrogen peroxide (H2O2) production, the performance of graphitic carbon nitride (g-C3N4) is curtailed by a central synthesis paradox: the mutually exclusive conditions required to simultaneously create its most effective dual active sites-nitrogen vacancies and cyano groups. Herein, this paradox is resolved with a molecular assembly-molten salt coupling strategy, a precise bottom-up approach enabling the one-step, synergistic creation of K-doped g-C3N4 with both defect types. This photocatalyst achieves an exceptional H2O2 production activity of 2.65 mmolg-1h-1, which is 6.2 and 3.0 times higher than that of pristine and physically-ground K-doped g-C3N4, respectively. Characterization and theoretical calculations reveal that molecular assembly promotes K+ interlayer embedding to facilitate charge migration, while the dual defects exhibit functional complementarity: nitrogen vacancies enhance O2 adsorption, and cyano groups facilitate proton coupling. In situ analysis also confirms an easier O2 activation effect and a lowered energy barrier for *OOH formation, ensuring high selectivity via a two-step, single-electron pathway. This study not only offers a route to rationally engineer dual-defect sites in carbon nitride but also provides a generalizable strategy for designing other advanced photocatalysts.