Electronic Structure Optimization and Proton-Transfer Enhancement on Titanium Oxide-Supported Copper Nanoparticles for Enhanced Nitrogen Recycling from Nitrate-Contaminated Water

Electrocatalytic reduction of nitrate to NH3 (NO3RR) on Cu offers sustainable NH3 production and nitrogen recycling from nitrate-contaminated water. However, Cu affords limited NO3RR activity owing to its unfavorable electronic state and the slow proton transfer on its surface, especially in neutral...

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Published in:Environmental science & technology 2023-07, Vol.57 (27), p.10117-10126
Main Authors: Liu, Zixun, Shen, Fei, Shi, Li, Tong, Qiuwen, Tang, Mu’e, Li, Yiming, Peng, Min, Jiao, Zhaojie, Jiang, Yan, Ao, Liang, Fu, Wenyang, Lv, Xiaoshu, Jiang, Guangming, Hou, Li’an
Format: Article
Language:English
Subjects:
Adsorbed water
adsorption
Ammonia
Catalysts
Chemical reduction
Contamination
Copper
copper nanoparticles
dissociation
electric field
Electric fields
Electron states
Electronic structure
environmental science
lakes
Leaching
Nanoparticles
Nitrates
Nitrates - chemistry
Nitrogen
Optimization
Physico-Chemical Treatment and Resource Recovery
Protons
Recycling
titanium
Titanium dioxide
Titanium oxide
Titanium oxides
Water
Water pollution
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Summary:Electrocatalytic reduction of nitrate to NH3 (NO3RR) on Cu offers sustainable NH3 production and nitrogen recycling from nitrate-contaminated water. However, Cu affords limited NO3RR activity owing to its unfavorable electronic state and the slow proton transfer on its surface, especially in neutral/alkaline media. Furthermore, although a synchronous “NO3RR and NH3 collection” system has been developed for nitrogen recycling from nitrate-laden water, no system is designed for natural water that generally contains low-concentration nitrate. Herein, we demonstrate that depositing Cu nanoparticles on a TiO2 support enables the formation of electron-deficient Cuδ+ species (0 < δ ≤ 2), which are more active than Cu0 in NO3RR. Furthermore, TiO2–Cu coupling induces local electric-field enhancement that intensifies water adsorption/dissociation at the interface, accelerating proton transfer for NO3RR on Cu. With the dual enhancements, TiO2–Cu delivers an NH3-N selectivity of 90.5%, mass activity of 41.4 mg-N h gCu –1, specific activity of 377.8 mg-N h–1 m–2, and minimal Cu leaching (
ISSN:0013-936X
1520-5851
1520-5851
DOI:10.1021/acs.est.3c03431