State Key Laboratory of Pollution Control and Resources Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China.
State Key Laboratory of Pollution Control and Resources Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China; Nanjing Innovation Center for Environmental Protection Industry, Nanjing 211106, PR China.
J Hazard Mater. 2020 Jul 5;393:122395. doi: 10.1016/j.jhazmat.2020.122395. Epub 2020 Feb 26.
Transition-metal catalysts (TMCs) for peroxymonosulfate (PMS) activation suffer from low stability (i.e. severe metal leakage and poor reusability) when maintaining high activity in water decontamination. An innovative carbonate (CO)-mediated method to synchronously enhance the catalytic activity and stability of TMCs was developed herein. In a model PMS/CoO nanowire system for bisphenol A (BPA) degradation, the first-order kinetic constant and total organic carbon removal ratio were increased by 202.27% and 71.32% upon adding CO, respectively. Meanwhile, the cobalt release amount was significantly reduced from 4.90 to 0.03 mg/L, and the number of reuse with high efficiency (>90% of BPA removal within 10 min) was augmented from 1 to 3 times. The CO buffered pH decline to repress metal leakage, and promoted Co(III) reduction into Co(II) to avoid the over-oxidation of catalyst. Under the driving of CO, the dominated reactive species were switched from •OH/SO to O accompanying the migration of catalytic center from Co(II) to Co(III). The Co(III) and CO/OH acted as electron and proton acceptors, respectively, to accelerate PMS decomposition into SO and subsequent generation of vast O. This work proposes a green way to construct novel O-based catalytic systems with excellent activity and stability for pollution remediation.
过渡金属催化剂(TMCs)在过一硫酸盐(PMS)激活中用于水净化时,存在活性高但稳定性差(即严重的金属泄漏和较差的可重复使用性)的问题。本文开发了一种创新的碳酸根(CO)介导的方法,可同时提高 TMCs 的催化活性和稳定性。在用于双酚 A(BPA)降解的 PMS/CoO 纳米线模型体系中,添加 CO 后,一级动力学常数和总有机碳去除率分别提高了 202.27%和 71.32%。同时,钴的释放量从 4.90 降至 0.03 mg/L,高效重复使用次数(10 min 内去除 BPA 超过 90%)从 1 次增加到 3 次。CO 缓冲 pH 值下降,抑制了金属泄漏,并促进了 Co(III)还原为 Co(II),从而避免了催化剂的过度氧化。在 CO 的驱动下,主导的活性物质从•OH/SO 转变为 O,同时催化中心从 Co(II)迁移到 Co(III)。Co(III)和 CO/OH 分别作为电子和质子受体,加速了 PMS 分解为 SO 和随后产生大量的 O。这项工作提出了一种构建具有优异活性和稳定性的新型基于 O 的催化体系的绿色方法,可用于污染修复。