College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China.
Changzhou Institute of Building Science, Changzhou, 213000, China.
Chemosphere. 2023 Oct;338:139540. doi: 10.1016/j.chemosphere.2023.139540. Epub 2023 Jul 21.
In the Fenton-like processes, the resources that exist in the system itself (e.g., dissolved oxygen, electron-rich pollutants) are often overlooked. Herein, a novel CuCo-LDO/CN composite catalyst with a strong "metal-π" effect was fabricated by in situ calcination which could activate dissolved oxygen to generate active oxygen species and degrade the electron-rich pollutants directly. The CuCo-LDO/CN (1:10) with the largest specific surface aera, most C-O-M bonds and least oxygen vacancies exhibited the best catalytic performance for tetracycline (TC)degradation (TC removal efficiency 93.2% and mineralization efficiency 40%, respectively, after 40 min at neutral pH) compared to CuCo-LDO and other CuCo-LDO/CN composite catalysts. In the absence of HO, dissolved oxygen could be activated by the catalyst to generate O·and ·OH, which contributed to approximately 20.7% of TC degradation, providing a faster and cost-effective way for TC removal from wastewater. While in the presence of HO, it was activated by CuCo-LDO/CN to generate·OH as the dominant reactive oxygen species and meanwhile TC transferred electrons to HO through C-O-M bonds, accelerating the Cu/Cu and Co/Co redox cycles. The possible degradation pathways of TC were proposed, and the environmental hazard of TC is greatly mitigated according to toxicity prediction.
在类 Fenton 过程中,系统本身存在的资源(例如溶解氧、富电子污染物)经常被忽视。在此,通过原位煅烧制备了一种具有强“金属-π”效应的新型 CuCo-LDO/CN 复合催化剂,它可以激活溶解氧来产生活性氧物种并直接降解富电子污染物。比表面积最大、C-O-M 键最多、氧空位最少的 CuCo-LDO/CN(1:10)在中性 pH 下 40 min 后对四环素(TC)的降解(TC 去除率为 93.2%,矿化率为 40%)表现出最好的催化性能,优于 CuCo-LDO 和其他 CuCo-LDO/CN 复合催化剂。在没有 HO 的情况下,催化剂可以激活溶解氧生成 O·和·OH,这对 TC 降解的贡献约为 20.7%,为废水去除 TC 提供了一种更快、更具成本效益的方法。而在有 HO 的情况下,它被 CuCo-LDO/CN 激活生成·OH 作为主要的活性氧物种,同时 TC 通过 C-O-M 键将电子转移给 HO,加速了 Cu/Cu 和 Co/Co 的氧化还原循环。提出了 TC 的可能降解途径,并根据毒性预测大大减轻了 TC 的环境危害。