Zeolitic imidazolate framework derived Fe catalyst electrocatalytic-driven atomic hydrogen for efficient reduction of nitrate to N2

Excessive discharge of nitrogen-containing chemical products into the natural water environment leads to the serious environmental problem of nitrate-nitrogen pollution, threatening the ecological balance and human health. In this study, we propose an efficient denitrification electrochemical method...

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Veröffentlicht in:Journal of hazardous materials 2024-06, Vol.471, p.134354-134354, Article 134354
Hauptverfasser: Ma, Xi, Zhong, Jiapeng, Wang, Rongyue, Li, Dexuan, Li, Kai, Luo, Lijun, Li, Chuanhao
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Sprache:eng
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Zusammenfassung:Excessive discharge of nitrogen-containing chemical products into the natural water environment leads to the serious environmental problem of nitrate-nitrogen pollution, threatening the ecological balance and human health. In this study, we propose an efficient denitrification electrochemical method utilizing iron-doped zeolite imidazolium framework derived defective nitrogen-doped carbon (d-FeNC) catalysts. The d-FeNC catalyst exhibited 97 % nitrate removal efficiency and 94 % total nitrogen (TN) removal, and the reaction rate constant was increased from 0.73 h−1 of the Fe-undoped electrocatalyst (d-NC) to 1.11 h−1. The successful synthesis of d-FeNC with carbon defect sites and encapsulated Fe was confirmed by in-depth characterization. In situ electron paramagnetic resonance (EPR) analysis in conjunction with cyclic voltammetry (CV) tests confirmed the carbon substrates with defect enhanced the trapping of atomic hydrogen (H*) on the catalyst surface. Density functional theory (DFT) calculations clarified the doping of Fe facilitated the adsorption of nitrate, resulting in contact of H* with nitrate on the catalyst surface. In the synergy of the defective state organic framework and metal Fe, H* and nitrate realized a collision process. The electrochemical denitrification system achieved an excellent nitrate removal capacity of 7587 mgN·g−1cat in high-concentration nitrate solution and showed excellent stability under various conditions. Overall, this study underscores the potential of defective iron-doped carbon catalysts for efficient electrocatalytic denitrification, providing a promising approach for sustainable wastewater treatment. [Display omitted] ●Electrocatalytic reduction of NO3− to N2 was achieved by iron-doped carbon catalysts (d-FeNC).●The defects of d-FeNC contributed to capture the atomic hydrogen.●Doping of Fe facilitated the adsorption of nitrate.●Electrocatalytic NO3− removal reached 93 % with d-FeNC in farm wastewater.
ISSN:0304-3894
1873-3336
DOI:10.1016/j.jhazmat.2024.134354