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

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中图分类号：0643 doi：10.1016/j.actphy.2025.100183

Ionic polarization engineering polymeric carbon nitride toward efficient H2O2 photosynthesis

Yao Xie ¹， Shuangjun Li2 ，Chao Chen¹，Siyu Fan ³， Ying Tao 1*， Qitao Zhang1* 1 International Collaborative Laboratory 2D Materials for Optoelectronic Science & ， Microscale Optoelectronics， Shenzhen University， Shenzhen 518060， Guangdong Province， China. ² Research Center Nano Science and ， Shanghai University， Shanghai 20o444， China. 3 ， ， ， ， .

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 polymeric carbon nitride （PCN）， fering 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 PCN，achieving two distinct crystalline phases： heptazine-dominated （LKCN-0.95）and heptazinetriazine 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+. -dominatedsystems enable triazine incorporation. The optimized heptazine-dominated and heptazine-triazine junction exhibited 27- fold and 42-fold enhancements in H2O2 photosynthesis （3.3 and 5.2mmolL-1h-1; ）compared to pristine PCN （0.12mmolL-1h-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 molten salt-driven structural evolution but also provides a scalable approach for designing efficient photocatalysts toward solar-driven H2O2 （204 photosynthesis.

Key Words： Polymeric carbon nitride； Heptazine-Triazine; Ionic polarization;Hydrogen peroxide; Photosynthesis

1引言

过氧化氢 （H2O2） 是一种重要的绿色化学品，在环境修复、化学合成和能源存储等多个领域具有广泛应用[1，2]。（剩余24154字）