Ma Chenwei, Xiao Quanxi, Wang Yufei, Zhou Yundi, Yang Zihe, Che Huinan
Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, No. 1, Xikang Road, Nanjing 210098, China.
Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, No. 1, Xikang Road, Nanjing 210098, China.
J Colloid Interface Sci. 2025 Jan 15;678(Pt C):180-190. doi: 10.1016/j.jcis.2024.09.118. Epub 2024 Sep 14.
Constructing a photocatalytic in-situ Fenton system (PISFs) is a promising strategy to address the need for continuous hydrogen peroxide (HO) addition and the low efficiency of HO activation for hydroxyl radical generation in the traditional Fenton reaction. In this study, we constructed a photocatalytic in-situ Fenton system using anthraquinone-modified carbon nitride (AQ-CN) for efficient pollutant degradation. The resultant AQ-CN not only enhanced the production of HO but also increased the generation of hydroxyl radical (·OH). Experimental results demonstrated that, the apparent rate constant for the degradation of 2,4-Dichlorophenol (2,4-DCP) by AQ-CN-PISFs was 0.145 min, which is 2.74 times higher than that of CN under visible light. Density functional theory (DFT) calculations indicate that AQ modification promotes electron-hole separation while increasing the adsorption energy of O. Independent gradient model (IGM) analysis based on Hirshfeld Partition revealed that van der Waals interactions between AQ-CN and 2,4-DCP promoted the degradation process. This work provides new ideas to overcome the problems of continuous addition of HO and low utilization of ·OH that exist in conventional Fenton system.
构建光催化原位芬顿体系（PISFs）是一种很有前景的策略，可满足传统芬顿反应中持续添加过氧化氢（HO）的需求以及HO活化生成羟基自由基效率较低的问题。在本研究中，我们构建了一种使用蒽醌修饰的氮化碳（AQ-CN）的光催化原位芬顿体系，用于高效降解污染物。所得的AQ-CN不仅提高了HO的产量，还增加了羟基自由基（·OH）的生成。实验结果表明，AQ-CN-PISFs降解2,4-二氯苯酚（2,4-DCP）的表观速率常数为0.145 min，在可见光下比CN高2.74倍。密度泛函理论（DFT）计算表明，AQ修饰促进了电子-空穴分离，同时增加了O的吸附能。基于Hirshfeld划分的独立梯度模型（IGM）分析表明，AQ-CN与2,4-DCP之间的范德华相互作用促进了降解过程。这项工作为克服传统芬顿体系中存在的HO持续添加问题和·OH利用率低的问题提供了新思路。
