Enhanced CO 2 Photoconversion Efficiency in Atomic Co Immobilized Covalent Organic Frameworks Heterostructure via Boosting Charge Dynamics and Active Site Accessibility

作者：Qi Li, Xiang Li, Fanqi Luo, Shan Hu, Mang Zheng, Qian Liu, Bin Zhang, Baojiang Jiang · 发表于：Small · 年份：2025 · DOI：10.1002/smll.202511246 · 被引用次数：2 · 研究领域：Covalent Organic Framework Applications、CO2 Reduction Techniques and Catalysts、Advanced Photocatalysis Techniques

Abstract Photocatalytic conversion of CO 2 into fuels and chemicals is of great significance for advancing sustainable development, yet its conversion efficiency remains constrained by inefficient charge separation and poor catalytic activity. Herein, a hybrid heterostructure is fabricated by in situ growth of bipyridine and triazine containing covalent organic frameworks (COFs) on SnS 2 nanosheets. Based on this heterostructure, a molecular engineering strategy is subsequently employed to design highly active single Co sites coordinated by bipyridine‐N motifs featuring distinctive electronic moieties. As a result, the optimized photocatalyst (SnS 2 /Co‐TAPT‐Bpy) enables an exceptional photocatalytic performance toward CO production under visible light irradiation with tunable CO/H 2 ration via changing the components of the heterojunctions. Experimental and theoretical investigations confirm that the photogenerated electrons can efficiently transfer from the SnS 2 component to the Co‐TAPT‐Bpy component through the interfacial electron field. More impressively, the electron‐deficient triazine motifs in Co‐TAPT‐BPy direct these photogenerated electrons toward the Co (II) active sites for CO 2 reduction. These atomically dispersed N‐Co‐N sites enhance CO 2 activation and protonation through d‐π orbital interactions, and suppress the competing H 2 evolution reaction, thus facilitating CO 2 conversion. This work highlights the potential of molecular regulation within heterojuncti...