Ternary Co…Ov…Cu sites trigger Co-utilization of endogenous electron donor-acceptor for sustainable removal of refractory low-carbon fatty amines in Fenton-like system

• Published in: Applied catalysis. B, Environmental Vol. 340; p. 123184
• Main Authors: Dai, Qin, Yu, Guangfei, Qi, Juanjuan, Wang, Yanan, Xing, Lei, Wang, Yihao, Zhang, Zhijie, Zhong, Xiaolin, Fang, Zhimo, Du, Penghui, Lyu, Lai, Wang, Lidong
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01-01-2024
• Subjects: Dimethylamine; Fenton-like reaction; O2 activation; Oxidant utilization efficiency; Ternary Co…Ov…Cu sites; Oxidant utilization efficiency; Dimethylamine; O2 activation; Ternary Co…Ov…Cu sites; Fenton-like reaction
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2023.123184

Herein, we fabricated CoCu-0.25-Ov with ternary Co…Ov…Cu sites through simple co-precipitation to achieve effective co-utilization of organics and dissolved oxygen (DO) as endogenous electron donor-acceptor in Fenton-like system. Around 100% of dimethylamine (DMA) min within 30 is removed. The involved kinetics (0.22 min−1) and oxidant utilization efficiency (22.5%) are higher than controls with binary sites. Multi-scaled characterizations and theoretical calculations reveal that electron-polarized Co…Ov…Cu sites facilitate co-activation of DMA and DO as electron donor-acceptor through increasing d-band center and lowering work function of catalyst. Meanwhile, ternary sites favor 1O2 and SO4•− generation, and shorten the migration distance of active species to pollutant, thus achieving excellent dual performance improvements. Semi-quantitative results of ESR indicate that DO activation and peroxymonosulfate (PMS) oxidation contribute about three-fourths and one-fourth to 1O2 production, respectively. This contribution provides a new and sustainable strategy for high-efficiency and oxidant-saving removal of refractory pollutants in the environment.
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•Co…Ov…Cu sites greatly improve removal performance of DMA and PMS utilization rate.•Ternary sites activate DMA and DO to replace PMS and favor the formation of ROSs.•Increased d-band center and lower work function of catalyst boost the co-activation.•DMA is removal by enhanced multipath (self-oxidation, 1O2 and SO4•− attacks).•O2 activation and PMS oxidation contribute 3/4 and 1/4 to 1O2 formation, respectively.