Chinese Academy of Sciences Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, 230026 Hefei, China.
Chinese Academy of Sciences Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, 230026 Hefei, China;
Proc Natl Acad Sci U S A. 2020 Dec 8;117(49):30966-30972. doi: 10.1073/pnas.2005035117. Epub 2020 Nov 23.
Organic Fenton-like catalysis has been recently developed for water purification, but redox-active compounds have to be ex situ added as oxidant activators, causing secondary pollution problem. Electrochemical oxidation is widely used for pollutant degradation, but suffers from severe electrode fouling caused by high-resistance polymeric intermediates. Herein, we develop an in situ organic Fenton-like catalysis by using the redox-active polymeric intermediates, e.g., benzoquinone, hydroquinone, and quinhydrone, generated in electrochemical pollutant oxidation as HO activators. By taking phenol as a target pollutant, we demonstrate that the in situ organic Fenton-like catalysis not only improves pollutant degradation, but also refreshes working electrode with a better catalytic stability. Both O nonradical and ·OH radical are generated in the anodic phenol conversion in the in situ organic Fenton-like catalysis. Our findings might provide a new opportunity to develop a simple, efficient, and cost-effective strategy for electrochemical water purification.
有机类芬顿催化最近已被开发用于水净化，但氧化还原活性化合物必须作为氧化剂激活剂进行原位添加，从而导致二次污染问题。电化学氧化广泛用于污染物降解，但由于高电阻聚合中间体引起的严重电极结垢而受到限制。在此，我们通过使用电化学污染物氧化过程中生成的氧化还原活性聚合物中间体（例如苯醌、对苯二酚和醌氢醌）原位生成有机类芬顿类似物催化，将 HO 激活剂。以苯酚作为目标污染物，我们证明了原位有机类芬顿类似物催化不仅提高了污染物的降解效率，而且还通过更好的催化稳定性来刷新工作电极。在原位有机类芬顿类似物催化中，阳极苯酚转化过程中同时生成了 O 非自由基和·OH 自由基。我们的研究结果可能为电化学水净化提供一种简单、高效和具有成本效益的策略。
