Highly selective urea electrooxidation coupled with efficient hydrogen evolution

Electrochemical urea oxidation offers a sustainable avenue for H 2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N 2 . Herein we demonstrate that atomically isolated...

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Published in	Nature communications Vol. 15; no. 1; pp. 5918 - 10
Main Authors	Zhan, Guangming, Hu, Lufa, Li, Hao, Dai, Jie, Zhao, Long, Zheng, Qian, Zou, Xingyue, Shi, Yanbiao, Wang, Jiaxian, Hou, Wei, Yao, Yancai, Zhang, Lizhi
Format	Journal Article
Language	English
Published	London Nature Publishing Group UK 14.07.2024 Nature Publishing Group Nature Portfolio
Subjects	119/118 140/133 140/146 140/58 639/301/299/886 639/638/161/886 639/638/169/896 Active sites Amino groups Asymmetry Carbonyl compounds Carbonyls Cyanates Denitrification Electrocatalysts Electrochemistry Evolution Humanities and Social Sciences Hydrogen evolution Hydrogen production multidisciplinary Nitrites Oxidation Photovoltaic cells Photovoltaics Science Science (multidisciplinary) Selectivity Solar energy Urea Wastewater
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Abstract	Electrochemical urea oxidation offers a sustainable avenue for H 2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N 2 . Herein we demonstrate that atomically isolated asymmetric Ni–O–Ti sites on Ti foam anode achieve a N 2 selectivity of 99%, surpassing the connected symmetric Ni–O–Ni counterparts in documented Ni-based electrocatalysts with N 2 selectivity below 55%, and also deliver a H 2 evolution rate of 22.0 mL h –1 when coupled to a Pt counter cathode under 213 mA cm –2 at 1.40 V RHE . 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 N 2 evolution. A prototype device powered by a commercial Si photovoltaic cell is further developed for solar-powered on-site urine processing and decentralized H 2 production. Urea electrooxidation often produces harmful cyanates and nitrites instead of N2, limiting its use in wastewater denitrification. Here, the authors develop an asymmetric Ni–O–Ti catalytic sites on Ti foam that reduce these byproducts, achieve 99% N2 selectivity, and boost H2 evolution.
AbstractList	Electrochemical urea oxidation offers a sustainable avenue for H 2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N 2 . Herein we demonstrate that atomically isolated asymmetric Ni–O–Ti sites on Ti foam anode achieve a N 2 selectivity of 99%, surpassing the connected symmetric Ni–O–Ni counterparts in documented Ni-based electrocatalysts with N 2 selectivity below 55%, and also deliver a H 2 evolution rate of 22.0 mL h –1 when coupled to a Pt counter cathode under 213 mA cm –2 at 1.40 V RHE . 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 N 2 evolution. A prototype device powered by a commercial Si photovoltaic cell is further developed for solar-powered on-site urine processing and decentralized H 2 production. Urea electrooxidation often produces harmful cyanates and nitrites instead of N2, limiting its use in wastewater denitrification. Here, the authors develop an asymmetric Ni–O–Ti catalytic sites on Ti foam that reduce these byproducts, achieve 99% N2 selectivity, and boost H2 evolution. 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. 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.Urea electrooxidation often produces harmful cyanates and nitrites instead of N2, limiting its use in wastewater denitrification. Here, the authors develop an asymmetric Ni–O–Ti catalytic sites on Ti foam that reduce these byproducts, achieve 99% N2 selectivity, and boost H2 evolution. Electrochemical urea oxidation offers a sustainable avenue for H production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N . Herein we demonstrate that atomically isolated asymmetric Ni-O-Ti sites on Ti foam anode achieve a N selectivity of 99%, surpassing the connected symmetric Ni-O-Ni counterparts in documented Ni-based electrocatalysts with N selectivity below 55%, and also deliver a H evolution rate of 22.0 mL h when coupled to a Pt counter cathode under 213 mA cm at 1.40 V . 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 N evolution. A prototype device powered by a commercial Si photovoltaic cell is further developed for solar-powered on-site urine processing and decentralized H production. 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.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. Electrochemical urea oxidation offers a sustainable avenue for H 2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N 2 . Herein we demonstrate that atomically isolated asymmetric Ni–O–Ti sites on Ti foam anode achieve a N 2 selectivity of 99%, surpassing the connected symmetric Ni–O–Ni counterparts in documented Ni-based electrocatalysts with N 2 selectivity below 55%, and also deliver a H 2 evolution rate of 22.0 mL h –1 when coupled to a Pt counter cathode under 213 mA cm –2 at 1.40 V RHE . 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 N 2 evolution. A prototype device powered by a commercial Si photovoltaic cell is further developed for solar-powered on-site urine processing and decentralized H 2 production.
ArticleNumber	5918
Author	Wang, Jiaxian Zhang, Lizhi Dai, Jie Hou, Wei Shi, Yanbiao Yao, Yancai Li, Hao Zheng, Qian Zhan, Guangming Zhao, Long Zou, Xingyue Hu, Lufa
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Snippet	Electrochemical urea oxidation offers a sustainable avenue for H 2 production and wastewater denitrification within the water-energy nexus; however, its wide... Electrochemical urea oxidation offers a sustainable avenue for H production and wastewater denitrification within the water-energy nexus; however, its wide... Electrochemical urea oxidation offers a sustainable avenue for H2 production and wastewater denitrification within the water-energy nexus; however, its wide... Abstract Electrochemical urea oxidation offers a sustainable avenue for H2 production and wastewater denitrification within the water-energy nexus; however,...
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SubjectTerms	119/118 140/133 140/146 140/58 639/301/299/886 639/638/161/886 639/638/169/896 Active sites Amino groups Asymmetry Carbonyl compounds Carbonyls Cyanates Denitrification Electrocatalysts Electrochemistry Evolution Humanities and Social Sciences Hydrogen evolution Hydrogen production multidisciplinary Nitrites Oxidation Photovoltaic cells Photovoltaics Science Science (multidisciplinary) Selectivity Solar energy Urea Wastewater
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Title	Highly selective urea electrooxidation coupled with efficient hydrogen evolution
URI	https://link.springer.com/article/10.1038/s41467-024-50343-8 https://www.ncbi.nlm.nih.gov/pubmed/39004672 https://www.proquest.com/docview/3080007823 https://www.proquest.com/docview/3080635267 https://pubmed.ncbi.nlm.nih.gov/PMC11247087 https://doaj.org/article/72927a905ef54936aad4b49eb3cbe8c7
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