物理化学学报2026，Vol.42Issue(5)：38-53,16.DOI:10.1016/j.actphy.2025.100183
离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成
Ionic polarization engineering of polymeric carbon nitride toward efficient H2O2 photosynthesis
摘要
Abstract
Molten salt polarization,leveraging ionic interactions in high-temperature molten salts,emerges as a powerful yet underexplored strategy for structural engineering.It enables precise structural engineering of polymeric carbon nitride(PCN),offering a promising strategy to boost photocatalytic H2O2 synthesis.Herein,we report a controlled modulation strategy by varying LiCl/KCl ratios in molten salts to tailor the framework structures of PCN,achieving two distinct crystalline phases:heptazine-dominated(LKCN-0.95)and heptazine-triazine donor-acceptor(D-A)junction(LKCN-0.2).By integrating experimental and theoretical analyses,we revealed that Li+-rich molten salts promote highly ordered heptazine frameworks,while K+-dominated systems enable triazine incorporation.The optimized heptazine-dominated and heptazine-triazine junction exhibited 27-fold and 42-fold enhancements in H2O2 photosynthesis(3.3 and 5.2 mmol L-1 h-1)compared to pristine PCN(0.12 mmol L-1 h-1),alongside exceptional stability over five cycles.Mechanistic studies demonstrated that structural modulation enhances charge separation and optimizes oxygen adsorption/activation for selective 2e-oxygen reduction.This work not only advances the understanding of molten salt-driven structural evolution but also provides a scalable approach for designing efficient photocatalysts toward solar-driven H2O2 photosynthesis.关键词
聚合碳氮化物/七嗪-三嗪/离子极化/过氧化氢/光合成Key words
Polymeric carbon nitride/Heptazine-Triazine/Ionic polarization/Hydrogen peroxide/Photosynthesis分类
化学化工引用本文复制引用
谢垚,李双军,陈超,樊思宇,陶英,张启涛..离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成[J].物理化学学报,2026,42(5):38-53,16.基金项目
本研究获得国家自然科学基金(22402122) （22402122）
国家博士后创新人才支持计划(GZC20231716) （GZC20231716）
广东省基础与应用基础研究基金(2024A1515010976) （2024A1515010976）
深圳市孔雀计划(20210802524B)及深圳市科技创新委员会(ZDSYS201707271014468)的资助. （20210802524B）
