Accelerated Fe2+ Regeneration in an Effective Electro-Fenton Process by Boosting Internal Electron Transfer to a Nitrogen-Conjugated Fe(III) Complex
- Mingyue LiuMingyue LiuSchool of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. ChinaMore by Mingyue Liu,
- Zhiyuan FengZhiyuan FengSchool of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. ChinaMore by Zhiyuan Feng,
- Xinmiao LuanXinmiao LuanState Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Siping Road 1239, Shanghai 200092, P. R. ChinaMore by Xinmiao Luan,
- Wenhai ChuWenhai ChuState Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Siping Road 1239, Shanghai 200092, P. R. ChinaMore by Wenhai Chu,
- Hongying Zhao*Hongying Zhao*Email: [email protected]. Tel.: +86-(0)21-65988570-8436. Fax: +86-(0)21-65982287School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, Tongji University, Siping Road 1239, Shanghai 200092, P. R. ChinaMore by Hongying Zhao, and
- Guohua Zhao
The regeneration rate of Fe2+ from Fe3+ dictates the performance of the electro-Fenton (EF) process, represented by the amount of produced hydroxyl radicals (·OH). Current strategies for the acceleration of Fe2+ regeneration normally require additional chemical reagents, to vary the redox potential of Fe2+/Fe3+. Here, we report an attempt at using the intrinsic property of the electrode to our advantage, i.e., nitrogen-doped carbon aerogel (NDCA), as a reducing agent for the regeneration of Fe2+ without using foreign reagents. Moreover, the pyrrolic N in NDCA provides unpaired electrons through the carbon framework to reduce Fe3+, while the graphitic and pyridinic N coordinate with Fe3+ to form a C–O–Fe–N2 bond, facilitating electron transfer from both the external circuit and pyrrolic N to Fe3+. Our Fe2+/NDCA-EF system exhibits a 5.8 ± 0.3 times higher performance, in terms of the amount of generated ·OH, than a traditional Fenton system using the same Fe2+ concentration. In the subsequent reaction, the Fe2+/NDCA-EF system demonstrates 100.0% removal of dimethyl phthalate, 3-chlorophenol, bisphenol A, and sulfamethoxazole with a low specific energy consumption of 0.17–0.36 kW·h·g–1. Furthermore, 90.1 ± 0.6% removal of dissolved organic carbon and 83.3 ± 0.9% removal of NH3-N are achieved in the treatment of domestic sewage. The purpose of this work is to present a novel strategy for the regeneration of Fe2+ in the EF process and also to elucidate the role of different N species of the carbonaceous electrode in contributing to the redox cycle of Fe2+/Fe3+.
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