Zeolitic imidazolate framework derived Fe catalyst electrocatalytic-driven atomic hydrogen for efficient reduction of nitrate to N2.
In: Journal of Hazardous Materials, Jg. 471 (2024-06-05), S. N.PAG
academicJournal
Zugriff:
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 NO 3 − to N 2 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 NO 3 − removal reached 93 % with d-FeNC in farm wastewater. [ABSTRACT FROM AUTHOR]
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Zeolitic imidazolate framework derived Fe catalyst electrocatalytic-driven atomic hydrogen for efficient reduction of nitrate to N2.
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Autor/in / Beteiligte Person: | Ma, Xi ; Zhong, Jiapeng ; Wang, Rongyue ; Li, Dexuan ; Li, Kai ; Luo, Lijun ; Li, Chuanhao |
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Zeitschrift: | Journal of Hazardous Materials, Jg. 471 (2024-06-05), S. N.PAG |
Veröffentlichung: | 2024 |
Medientyp: | academicJournal |
ISSN: | 0304-3894 (print) |
DOI: | 10.1016/j.jhazmat.2024.134354 |
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