Highly selective urea electrooxidation coupled with efficient hydrogen evolution

Guangming Zhan, Lufa Hu, Hao Li (), Jie Dai, Long Zhao, Qian Zheng, Xingyue Zou, Yanbiao Shi, Jiaxian Wang, Wei Hou, Yancai Yao () and Lizhi Zhang ()
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Guangming Zhan: Shanghai Jiao Tong University
Lufa Hu: Shanghai Jiao Tong University
Hao Li: Shanghai Jiao Tong University
Jie Dai: Shanghai Jiao Tong University
Long Zhao: Shanghai Jiao Tong University
Qian Zheng: Shanghai Jiao Tong University
Xingyue Zou: Shanghai Jiao Tong University
Yanbiao Shi: Shanghai Jiao Tong University
Jiaxian Wang: Shanghai Jiao Tong University
Wei Hou: Shanghai Jiao Tong University
Yancai Yao: Shanghai Jiao Tong University
Lizhi Zhang: Shanghai Jiao Tong University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Electrochemical urea oxidation offers a sustainable avenue for H2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N2. Herein we demonstrate that atomically isolated asymmetric Ni–O–Ti sites on Ti foam anode achieve a N2 selectivity of 99%, surpassing the connected symmetric Ni–O–Ni counterparts in documented Ni-based electrocatalysts with N2 selectivity below 55%, and also deliver a H2 evolution rate of 22.0 mL h–1 when coupled to a Pt counter cathode under 213 mA cm–2 at 1.40 VRHE. These asymmetric sites, featuring oxygenophilic Ti adjacent to Ni, favor interaction with the carbonyl over amino groups in urea, thus preventing premature resonant C⎓N bond breakage before intramolecular N–N coupling towards N2 evolution. A prototype device powered by a commercial Si photovoltaic cell is further developed for solar-powered on-site urine processing and decentralized H2 production.

Date: 2024
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DOI: 10.1038/s41467-024-50343-8

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