Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China; School of Materials Science and Engineering, Hebei University of Technology, Tianjin, 300401, China.
School of Chemical and Environmental Engineering, China University of Mining & Technology, Beijing, 100091, China.
Chemosphere. 2024 Jan;347:140620. doi: 10.1016/j.chemosphere.2023.140620. Epub 2023 Nov 15.
In this study, a heterogeneous photo-Fenton catalyst of Fe species/resorcinol-formaldehyde (Fe/RF) was synthesized in the degradation process of phenols under visible light in a homogeneous photo-Fenton system. The in situ generated HO by bare RF in the medium and the follow-added Fe can construct homogeneous photo-Fenton system, and Fe/RF heterogeneous photo-Fenton catalyst was formed after the reaction through Fe species self-deposition. Due to the addition of Fe, more hydroxyl radical (·OH) generated in the homogeneous Fenton system, which lead to the higher degradation efficiency of phenols that achieved 90.5 % with 150 min. Fe/RF was subsequently formed and more C=O functional group in the structure appeared, which was beneficial to the production of HO. The above-mentioned results can be proved by the involved calculation and experimental results. Fe species, including Fe and Fe, were beneficial to the conversion of reactive oxygen species (ROSs), and further improved the degradation efficiency of Phenols. Since the existence of photo-generated electrons, Fe concentration in the solution can maintain a stable level. Interestingly, the degradation efficiency of Phenols was higher when Fe was used instead of Fe as the additive, which may be caused by the promotive effect of Fe on singlet oxygen (O) generation. In addition, the degradation efficiency of Phenols under alkaline conditions was higher than that under acid conditions, which broke the limit of traditional Fenton process that works mostly in acidic medium. This study shows promising results in terms of synergistic photocatalytic/photo-Fenton processes for the degradation of organic pollutants in water.
在这项研究中，在均相光芬顿体系中可见光下酚类降解过程中，合成了一种 Fe 物种/间苯二酚-甲醛（Fe/RF）的非均相光芬顿催化剂。在介质中裸 RF 原位生成的 HO 和随后添加的 Fe 可以构建均相光芬顿体系，反应后通过 Fe 物种自沉积形成 Fe/RF 非均相光芬顿催化剂。由于 Fe 的添加，在均相 Fenton 体系中产生了更多的羟基自由基（·OH），导致酚类的降解效率更高，达到 90.5%，反应时间为 150 分钟。随后形成了 Fe/RF，结构中出现了更多的 C=O 官能团，有利于 HO 的生成。上述结果可以通过相关计算和实验结果得到证明。Fe 物种，包括 Fe 和 Fe，有利于活性氧物质（ROSs）的转化，进一步提高了酚类的降解效率。由于光生电子的存在，溶液中的 Fe 浓度可以保持稳定水平。有趣的是，当使用 Fe 代替 Fe 作为添加剂时，酚类的降解效率更高，这可能是因为 Fe 对单重态氧（O）生成的促进作用。此外，在碱性条件下酚类的降解效率高于酸性条件下的降解效率，打破了传统 Fenton 工艺主要在酸性介质中工作的限制。这项研究在协同光催化/光芬顿过程降解水中有机污染物方面显示出了有前景的结果。
