Inorganic Chemistry Communications ( IF 4.4 ) Pub Date : 2023-01-10 , DOI: 10.1016/j.inoche.2023.110396 Ziqin Xing , Meng Fan , Jianxin Liu , Yawen Wang , Xiaochao Zhang , Rui Li , Yunfang Wang , Caimei Fan
A low-cost and highly efficient Fenton-like catalyst desired to produce the hydroxyl radical (·OH) and sulfate radical (SO4·-) at the same time for environmental applications was successfully fabricated via a noval alcohol-thermal method. Remarkably, the Mn3O4/λ-MnO2 composite exhibited the highly efficient activation for peroxymonosulfate (PMS) and deep mineralization for phenol under visible-light irradiation. The phenol degradation fitted the pseudo-first-order reaction kinetics well with rate constant of 0.0455 min−1 for photo-Fenton-like system and 0.0340 min−1 for Fenton-like system, respectively. Based on the results of radical quantification experiments and electron spin resonance (ESR) tests, ·OH, SO4·- and superoxide radical (·O2–) species played imperative roles during the oxidation process. The active species were mainly derived from the multivalent manganese ions on the surface of Mn3O4/λ-MnO2 composite formed a cyclic loop and reacted with HSO5- of PMS, thus significantly enhancing the catalytic performance. Finally, the probable reaction mechanism of Mn3O4/λ-MnO2 catalyst activation of PMS in a Fenton-like system under solar irradiation or in dark were speculated. This work will provide a new idea for the practical application of PMS activation in the treatment of organic matters in the wastewater under solar light irradiation.
中文翻译:
一种新型类芬顿催化剂和过氧单硫酸盐活化剂 Mn3O4/λ-MnO2 的苯酚降解:协同效应和机理
通过一种新型醇热法成功制备了一种低成本、高效的类芬顿催化剂,可同时产生羟基自由基( · OH)和硫酸根(SO 4 · - ),用于环境应用。值得注意的是,Mn 3 O 4 / λ -MnO 2复合材料在可见光照射下表现出对过氧单硫酸盐 (PMS) 的高效活化和对苯酚的深度矿化。苯酚降解符合伪一级反应动力学,光芬顿类系统的速率常数为 0.0455 min -1 ,而 0.0340 min -1分别用于类芬顿系统。基于自由基量化实验和电子自旋共振(ESR)测试的结果,· OH、SO 4 · -和超氧自由基(· O 2 -)物种在氧化过程中起着不可或缺的作用。活性物种主要来源于Mn 3 O 4 / λ -MnO 2复合材料表面的多价锰离子形成循环环与PMS的HSO 5 -反应,从而显着提高催化性能。最后,Mn 3 O 4的可能反应机理/ λ -MnO 2催化剂在太阳辐射或黑暗条件下类芬顿体系中 PMS 的活化被推测。该工作将为PMS活化在太阳光照射下废水中有机物处理的实际应用提供新思路。