School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.
Chemosphere. 2022 Mar;291(Pt 3):133039. doi: 10.1016/j.chemosphere.2021.133039. Epub 2021 Nov 22.
This study fabricated an efficient P and Fe co-doping graphitic carbon nitride catalyst (Fe- CN/P) by thermal polymerization of melamine, FeCl, and 2-hydroxyphosphonoacetic acid (HPAA) mixture. The Fe-CN/P catalyst exhibited much better tetracycline hydrochloride (TCH) degradation performance than that of single doping and neat CN. Various characterizations indicated that the introduction of HPAA significantly increased the specific surface area of CN and improved charge separation as well as transfer efficiency. Based on Fe 2p XPS analysis and indirect determination of hydroxyl radical (·OH) content, the separated photogenerated electrons accelerated the reduction of Fe(III) and activated photo-Fenton reaction, resulting in more ·OH species generation. The effect of pH value, catalyst dosages, HO concentration, the type of cations and anions as well as water matrices on the degradation of TCH by Fe-CN/P was systematically investigated. The main degradation pathways of TCH were proposed according to the LC-MS intermediates detection and DFT calculation. The results indicated that reactive oxide species (ROS) were more likely to attack the atoms with high Fukui index (f). This work provides new ideas for adjusting the morphology and electronic structure of CN to enhance its photo-Fenton catalytic activity.
本研究通过三聚氰胺、FeCl3 和 2-羟基亚磷酸混合物的热聚合制备了一种高效的 P 和 Fe 共掺杂石墨相氮化碳催化剂（Fe-CN/P）。Fe-CN/P 催化剂对盐酸四环素（TCH）的降解性能明显优于单掺杂和纯 CN。各种表征表明，HPAA 的引入显著提高了 CN 的比表面积，并改善了电荷分离和转移效率。基于 Fe 2p XPS 分析和羟基自由基（·OH）含量的间接测定，分离的光生电子加速了 Fe(III)的还原和光芬顿反应的激活，导致更多的·OH 生成。系统研究了 pH 值、催化剂用量、HO 浓度、阳离子和阴离子的类型以及水基质对 Fe-CN/P 降解 TCH 的影响。根据 LC-MS 中间体检测和 DFT 计算提出了 TCH 的主要降解途径。结果表明，活性氧化物（ROS）更有可能攻击富 Fukui 指数（f）的原子。这项工作为调整 CN 的形态和电子结构以提高其光芬顿催化活性提供了新的思路。
