Liu Mengting, Zhang Wanyu, Ni Ruiting, Wang Zhenxiao, Zhao Hongyao, Zhong Xiu, Wang Yanyun, Shang Danhong, Guo Zengjing, Ang Edison Huixiang, Yang Fu
School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, Jiangsu, P. R. China.
School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252000, Shandong, P. R. China.
Mater Horiz. 2024 Jul 15;11(14):3316-3329. doi: 10.1039/d4mh00285g.
Wastewater treatment recycling is critical to ensure safe water supply or to overcome water shortage. Herein, we developed metallic Co integration onto MnO nanorods (MON) resulting in a phase-separated synergetic catalyst by creating more Mn(III) the Jahn-Teller effect and oxygen vacancies and improving the redox capability of Co nanoparticles mediated by a thin carbon layer. Additionally, the N-doped surface carbon network on MON contributes to polar sites, facilitating the enrichment of contaminants around reactive sites, thereby shortening the migration of reactive oxidative species (ROS) toward contaminants. The optimized MnO@Co/C-600 exhibits superior PMS activation efficiency for bisphenol A degradation (0.463 min), displaying nearly a 20-fold enhancement in the rate constant compared to MnO/C-600. Subsequent experiments involving variable modulation and extension were conducted to further elucidate the multiple synergistic effects. The mechanism study further confirms the synergy of ˙SO, ˙OH, ˙O, and O, along with additional electron transfer pathways. The intermediates generated during degradation pathways and their toxicity to aquatic organisms were identified. Notably, a monolith integrated catalyst was explored by anchoring MnO@Co/C-600 onto a tailored melamine sponge based on Ca ion triggered crosslink tactic for the photothermal degradation of bisphenol A, tetracycline and norfloxacin, endowed with easy recovery and good stability. Furthermore, we demonstrated that the total organic carbon removal of multiple contaminants surpassed that of sole contaminants.
废水处理循环利用对于确保安全供水或克服水资源短缺至关重要。在此,我们通过产生更多的Mn(III)( Jahn-Teller效应和氧空位)并提高由薄碳层介导的Co纳米颗粒的氧化还原能力,将金属Co整合到MnO纳米棒(MON)上,从而形成了一种相分离的协同催化剂。此外,MON上的N掺杂表面碳网络有助于形成极性位点,促进污染物在反应位点周围的富集,从而缩短反应性氧化物种(ROS)向污染物的迁移距离。优化后的MnO@Co/C-600对双酚A降解表现出卓越的PMS活化效率(0.463 min),与MnO/C-600相比,其速率常数提高了近20倍。随后进行了涉及变量调制和扩展的实验,以进一步阐明多种协同效应。机理研究进一步证实了˙SO、˙OH、˙O和O的协同作用以及额外的电子转移途径。确定了降解途径中产生的中间体及其对水生生物的毒性。值得注意的是,基于Ca离子触发的交联策略,通过将MnO@Co/C-600锚定在定制的三聚氰胺海绵上,探索了一种整体式集成催化剂,用于双酚A、四环素和诺氟沙星的光热降解,该催化剂具有易于回收和良好的稳定性。此外,我们证明了多种污染物的总有机碳去除率超过了单一污染物的去除率。