Spin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia

Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polari...

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Published inNature communications Vol. 15; no. 1; pp. 88 - 11
Main Authors Dai, Jie, Tong, Yawen, Zhao, Long, Hu, Zhiwei, Chen, Chien-Te, Kuo, Chang-Yang, Zhan, Guangming, Wang, Jiaxian, Zou, Xingyue, Zheng, Qian, Hou, Wei, Wang, Ruizhao, Wang, Kaiyuan, Zhao, Rui, Gu, Xiang-Kui, Yao, Yancai, Zhang, Lizhi
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 02.01.2024
Nature Publishing Group
Nature Portfolio
Subjects
119/118
140/131
140/146
140/58
147/137
639/301/299
639/638/161/886
704/172/169/896
Ammonia
Clean energy
Clean technology
Electrocatalysts
Electrochemistry
Electrode polarization
Electrodes
Electron spin
Humanities and Social Sciences
Hydrogenation
Intermediates
multidisciplinary
Nitrate reduction
Nitrates
Oxygen
Polarization (spin alignment)
Recovery
Renewable energy
Science
Science (multidisciplinary)
Sustainability
Sustainable development
Titanium
Wastewater treatment
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Abstract Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polarized Fe 1 −Ti pairs on monolithic titanium electrode that exhibits an attractive NH 3 yield rate of 272,000 μg h −1 mg Fe −1 and a high NH 3 Faradic efficiency of 95.2% at −0.4 V vs. RHE, far superior to the counterpart with spin−depressed Fe 1 −Ti pairs (51000 μg h –1 mg Fe –1 ) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow−through electrolyzer with a membrane-based NH 3 recovery unit, the simultaneous nitrate reduction and NH 3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment. Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production. Here, the authors construct spin−polarized Fe 1 −Ti pairs via manipulating oxygen vacancies on monolithic titanium electrode for highly efficient nitrate to ammonia conversion.
AbstractList Abstract Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polarized Fe1−Ti pairs on monolithic titanium electrode that exhibits an attractive NH3 yield rate of 272,000 μg h−1 mgFe −1 and a high NH3 Faradic efficiency of 95.2% at −0.4 V vs. RHE, far superior to the counterpart with spin−depressed Fe1−Ti pairs (51000 μg h–1 mgFe –1) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow−through electrolyzer with a membrane-based NH3 recovery unit, the simultaneous nitrate reduction and NH3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment.
Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polarized Fe1−Ti pairs on monolithic titanium electrode that exhibits an attractive NH3 yield rate of 272,000 μg h−1 mgFe−1 and a high NH3 Faradic efficiency of 95.2% at −0.4 V vs. RHE, far superior to the counterpart with spin−depressed Fe1−Ti pairs (51000 μg h–1 mgFe–1) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow−through electrolyzer with a membrane-based NH3 recovery unit, the simultaneous nitrate reduction and NH3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment.Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production. Here, the authors construct spin−polarized Fe1−Ti pairs via manipulating oxygen vacancies on monolithic titanium electrode for highly efficient nitrate to ammonia conversion.
Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin-state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin-polarized Fe1-Ti pairs on monolithic titanium electrode that exhibits an attractive NH3 yield rate of 272,000 μg h-1 mgFe-1 and a high NH3 Faradic efficiency of 95.2% at -0.4 V vs. RHE, far superior to the counterpart with spin-depressed Fe1-Ti pairs (51000 μg h-1 mgFe-1) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow-through electrolyzer with a membrane-based NH3 recovery unit, the simultaneous nitrate reduction and NH3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment.Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin-state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin-polarized Fe1-Ti pairs on monolithic titanium electrode that exhibits an attractive NH3 yield rate of 272,000 μg h-1 mgFe-1 and a high NH3 Faradic efficiency of 95.2% at -0.4 V vs. RHE, far superior to the counterpart with spin-depressed Fe1-Ti pairs (51000 μg h-1 mgFe-1) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow-through electrolyzer with a membrane-based NH3 recovery unit, the simultaneous nitrate reduction and NH3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment.
Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polarized Fe 1 −Ti pairs on monolithic titanium electrode that exhibits an attractive NH 3 yield rate of 272,000 μg h −1 mg Fe −1 and a high NH 3 Faradic efficiency of 95.2% at −0.4 V vs. RHE, far superior to the counterpart with spin−depressed Fe 1 −Ti pairs (51000 μg h –1 mg Fe –1 ) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow−through electrolyzer with a membrane-based NH 3 recovery unit, the simultaneous nitrate reduction and NH 3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment.
Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin–state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin−polarized Fe 1 −Ti pairs on monolithic titanium electrode that exhibits an attractive NH 3 yield rate of 272,000 μg h −1 mg Fe −1 and a high NH 3 Faradic efficiency of 95.2% at −0.4 V vs. RHE, far superior to the counterpart with spin−depressed Fe 1 −Ti pairs (51000 μg h –1 mg Fe –1 ) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow−through electrolyzer with a membrane-based NH 3 recovery unit, the simultaneous nitrate reduction and NH 3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment. Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production. Here, the authors construct spin−polarized Fe 1 −Ti pairs via manipulating oxygen vacancies on monolithic titanium electrode for highly efficient nitrate to ammonia conversion.
ArticleNumber 88
Author Gu, Xiang-Kui
Zhang, Lizhi
Yao, Yancai
Chen, Chien-Te
Hu, Zhiwei
Zhao, Long
Zou, Xingyue
Wang, Kaiyuan
Wang, Jiaxian
Dai, Jie
Kuo, Chang-Yang
Hou, Wei
Tong, Yawen
Zheng, Qian
Zhan, Guangming
Wang, Ruizhao
Zhao, Rui
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Snippet Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the...
Abstract Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers...
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Ammonia
Clean energy
Clean technology
Electrocatalysts
Electrochemistry
Electrode polarization
Electrodes
Electron spin
Humanities and Social Sciences
Hydrogenation
Intermediates
multidisciplinary
Nitrate reduction
Nitrates
Oxygen
Polarization (spin alignment)
Recovery
Renewable energy
Science
Science (multidisciplinary)
Sustainability
Sustainable development
Titanium
Wastewater treatment
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Title Spin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia
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