College of Environmental Science and Engineering, Beijing Forestry University, Beijing, 100083, PR China.
College of Environmental Science and Engineering, Beijing Forestry University, Beijing, 100083, PR China.
Environ Res. 2022 Nov;214(Pt 3):114065. doi: 10.1016/j.envres.2022.114065. Epub 2022 Aug 11.
The present work demonstrates a simple one-step pyrolysis method for the synthesis of a catalytic sludge-based carbon (SBC) biochar containing Fe and Mn from dehydrated sludge with added KMnO and Fe(II). The electrocatalytic degradation of triclosan (TCS) in water was evaluated using an Fe/Mn-SBC cathode to promote a heterogeneous Fenton-like reaction. The catalyst generated at 500 °C exhibited an abundant porous structure and a relatively high surface area, and produced an electrode with better conductivity and electron diffusion. The presence of metal oxides changed the surface structure defects of this biochar and enhanced its catalytic performance while increasing the electrochemically active surface area by 72.68 mF/cm compared with plain SBC. TCS was degraded (91.3%) within 180 min by oxygen species generated in situ on an Fe/Mn-SBC cathode because the activation energy for oxygen reduction was lowered by 4.62 kJ/mol. The degradation of TCS followed pseudo first-order kinetics and was controlled by TCS diffusion and interfacial chemical reactions between adsorbed TCS and the electrode. Possible TCS degradation pathways were devised based on the main intermediates, and O was found to be more important than •OH radicals. Through toxicity test and prediction, the toxicity of degradation was gradually reduced. This study demonstrates a simple and ecofriendly method for the electrocatalytic degradation of organic pollutants.
本工作展示了一种简单的一步热解方法,用于从脱水污泥中合成含有 Fe 和 Mn 的催化污泥基碳(SBC)生物炭,该污泥中添加了 KMnO 和 Fe(II)。使用 Fe/Mn-SBC 阴极来促进非均相类芬顿反应,评估了三氯生(TCS)在水中的电催化降解。在 500°C 下生成的催化剂具有丰富的多孔结构和较高的比表面积,生成的电极具有更好的导电性和电子扩散性。金属氧化物的存在改变了这种生物炭的表面结构缺陷,提高了其催化性能,同时与普通 SBC 相比,增加了 72.68 mF/cm 的电化学活性表面积。由于氧还原的活化能降低了 4.62 kJ/mol,因此在 Fe/Mn-SBC 阴极原位生成的氧物种作用下,TCS 在 180 min 内降解了 91.3%。TCS 的降解遵循拟一级动力学,受 TCS 扩散和吸附 TCS 与电极之间的界面化学反应控制。根据主要中间体设计了可能的 TCS 降解途径,并发现 O 比 •OH 自由基更重要。通过毒性测试和预测,降解的毒性逐渐降低。本研究展示了一种简单且环保的电催化降解有机污染物的方法。