Cu1-Fe Dual Sites for Superior Neutral Ammonia Electrosynthesis from Nitrate

被引：69

作者：

Zhou, Biao ^{[1
]}

Yu, Linghao ^{[1
]}

Zhang, Weixing ^{[1
]}

Liu, Xupeng ^{[1
]}

Zhang, Hao ^{[1
]}

Cheng, Jundi ^{[1
]}

Chen, Ziyue ^{[1
]}

Li, Meiqi ^{[2
]}

Shi, Yanbiao ^{[2
]}

Jia, Falong ^{[1
]}

Huang, Yi ^{[1
]}

Zhang, Lizhi ^{[2
]}

Ai, Zhihui ^{[1
]}

机构：

[1] Cent China Normal Univ, Coll Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control, Inst Environm & Appl Chem,Minist Educ,Key Lab Pes, Wuhan 430079, Peoples R China

[2] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2024年 / 63卷 / 31期

基金：

中国国家自然科学基金;

关键词：

Nitrate Electroreduction; Single Atom Copper; Dual sites; Nitrate-pollution Treatment; Ammonia Recovery; REDUCTION; CATALYSTS; CARBON; ELECTROREDUCTION; VACANCY;

D O I：

10.1002/anie.202406046

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The electrochemical nitrate reduction reaction (NO3RR) is able to convert nitrate (NO3-) into reusable ammonia (NH3), offering a green treatment and resource utilization strategy of nitrate wastewater and ammonia synthesis. The conversion of NO3- to NH3 undergoes water dissociation to generate active hydrogen atoms and nitrogen-containing intermediates hydrogenation tandemly. The two relay processes compete for the same active sites, especially under pH-neutral condition, resulting in the suboptimal efficiency and selectivity in the electrosynthesis of NH3 from NO3-. Herein, we constructed a Cu-1-Fe dual-site catalyst by anchoring Cu single atoms on amorphous iron oxide shell of nanoscale zero-valent iron (nZVI) for the electrochemical NO3RR, achieving an impressive NO3- removal efficiency of 94.8 % and NH3 selectivity of 99.2 % under neutral pH and nitrate concentration of 50 mg L-1 NO3--N conditions, greatly surpassing the performance of nZVI counterpart. This superior performance can be attributed to the synergistic effect of enhanced NO3- adsorption on Fe sites and strengthened water activation on single-atom Cu sites, decreasing the energy barrier for the rate-determining step of *NO-to-*NOH. This work develops a novel strategy of fabricating dual-site catalysts to enhance the electrosynthesis of NH3 from NO3-, and presents an environmentally sustainable approach for neutral nitrate wastewater treatment.

引用

页数：10

共 81 条

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