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

Jie Dai, Yawen Tong, Long Zhao, Zhiwei Hu, Chien-Te Chen, Chang-Yang Kuo, Guangming Zhan, Jiaxian Wang, Xingyue Zou, Qian Zheng, Wei Hou, Ruizhao Wang, Kaiyuan Wang, Rui Zhao, Xiang-Kui Gu (), Yancai Yao () and Lizhi Zhang ()
Additional contact information
Jie Dai: Shanghai Jiao Tong University
Yawen Tong: Wuhan University
Long Zhao: Shanghai Jiao Tong University
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Chien-Te Chen: National Synchrotron Radiation Research Center
Chang-Yang Kuo: National Synchrotron Radiation Research Center
Guangming Zhan: Shanghai Jiao Tong University
Jiaxian Wang: Shanghai Jiao Tong University
Xingyue Zou: Shanghai Jiao Tong University
Qian Zheng: Shanghai Jiao Tong University
Wei Hou: Shanghai Jiao Tong University
Ruizhao Wang: Shanghai Jiao Tong University
Kaiyuan Wang: Shanghai Jiao Tong University
Rui Zhao: Shanghai Jiao Tong University
Xiang-Kui Gu: Wuhan University
Yancai Yao: Shanghai Jiao Tong University
Lizhi Zhang: Shanghai Jiao Tong University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-023-44469-4

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