岛状单原子钴催化剂调制电荷捕获以增强类光芬顿反应,Advanced Functional Materials

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岛状单原子钴催化剂调制电荷捕获以增强类光芬顿反应
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-01-06 , DOI: 10.1002/adfm.202208688
Mengying Qian ₁ , Xi‐Lin Wu ₁ , Meichi Lu ₁ , Lizhou Huang ₁ , Wenxuan Li ₁ , Hongjun Lin ₁ , Jianrong Chen ₁ , Shaobin Wang ₂ , Xiaoguang Duan ₂

Affiliation

基于复合材料的光催化依赖于金属助催化剂和光敏剂（半导体）之间的界面电子转移来实现电荷载流子的空间分离。_{在此，构建了 Co-CN 单原子催化剂 (SAC) 和 gC 3} N ₄之间的巧妙异质结，用于异相类光芬顿反应。_{在跨异质结的内置电场的驱动下，光生电荷载流子的分离和迁移得到促进，导致电子从 gC 3} N ₄快速转移到 Co-CN SAC。理论计算和瞬态吸收光谱揭示了 SA-Co-CN/gC ₃ N _{4中的调制电荷转移和俘获}异质结构，导致在光照射下通过过氧单硫酸盐活化显着增强活性氧的产生。这种巧妙的 SA-Co-CN/gC ₃ N ₄ /PMS/vis 系统可有效氧化各种抗生素，具有高去除效率 (>98%)、宽操作 pH 范围 (pH 3–11) 和出色的稳定性长期经营。这项研究为基于 SAC 的异质结的合理设计提供了一种新策略，以桥接光催化和多相催化，通过界面耦合获得优异的光氧化还原活性。

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Modulation of Charge Trapping by Island-like Single-Atom Cobalt Catalyst for Enhanced Photo-Fenton-Like reaction

Composites-based photocatalysis relies on the interfacial electron transfer between the metallic cocatalyst and photosensitizer (the semiconductor) to realize spatial separation of charge carriers. Herein, an ingenious heterojunction between Co-CN single atom catalysts (SACs) and g-C₃N₄ is constructed for heterogeneous photo-Fenton-like reactions. Driven by built-in electric field across the heterojunctions, the separation and migration of the photogenerated charge carriers is promoted, leading to the fast electron transfer from the g-C₃N₄ to the Co-CN SACs. Theoretical calculations and transient absorption spectroscopy reveal the modulated charge transfer and trapping in the SA-Co-CN/g-C₃N₄ heterostructure, resulting in the remarkably enhanced generation of reactive oxygen species via peroxymonosulfate activation under light irradiation. This ingenious SA-Co-CN/g-C₃N₄/PMS/vis system is efficient for the oxidation of various antibiotics with high removal efficiency (>98%), a wide operating pH range (pH 3–11) and excellent stability in long-term operation. This study provides a new tactic for rational design of SACs-based heterojunctions to bridge photocatalysis and heterogeneous catalysis, attaining superior photoredox activity via interfacial coupling.

更新日期：2023-01-06

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