Li Gong,Leben Qiu,Xiaoqian Xing,Jieyun Zhu,Mengzhi Lu,Feier Dong,Yan Yu,Weiting Yu
Selectively reducing nitroaromatics into aromatic amines will not only remove nitroaromatic pollutants in waste effluents to reduce environmental risks, but also yield important feedstocks for chemical industrial manufactures. In this study, a FeCo-co-embedded N-doped Carbon (FeCo-N-C) catalyst with Fe-Co atomic pair has been identified with favorable activity, superior selectivity , excellent reusability, as well as outstanding performance in the treatment of real water. The combined results from theoretical study and experimental tests indicate that the improved catalytic performance of FeCo-N-C is owing to the narrowed band gap and electron delocalization caused by the Fe-Co atomic pair which can improve electron transport in its catalytic reaction. The results of isotope experiments and H* quenching experiments confirm that H 2 O is the source of hydrogen in catalytic reduction of PNP. FeCo-N-C is identified as a superior catalyst to replace multitudinous currently used noble-metal catalysts for the selective catalytic reduction of nitroaromatics in wastewater treatment .
Zhendong Zhao,Wenjun Zhou,Daohui Lin,Lizhong Zhu,Baoshan Xing,Zhiqi Liu
High metal loading of single-atom catalysts enables excellent catalytic activity, but possibly causes serious aggregation problem. Herein, a series of diatomic FeCo−N/C-x (x represents metal content) were skillfully designed and applied to improve the catalytic activity for peroxymonosulfate (PMS) activation toward degrading organic micropollutants. The unprecedented dual active sites, referring to Fe(N 3 )−Co(N 3 ) moiety and FeCo alloy, are constructed on the obtained FeCo−N/C-x, thereby exhibiting significantly greater performance toward degrading aqueous phenol (e.g., 0.316 min −1 for FeCo−N/C-3) via PMS activation, compared with those of traditional single-atom Co−N/C (0.011 min −1 ) and Fe−N/C (0.018 min −1 ). Combined experimental and theoretical calculations demonstrate the independent functions of dual active sites, in which Fe(N 3 )−Co(N 3 ) and FeCo alloy can decrease the energy barrier of O−O bond cleaving resulting in the formation of high-valent FeCo O reactive species and singlet oxygen, respectively. This study opens up a new platform toward constructing dual active sites for enhanced Fenton-like catalytic activity.
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