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

Author

Listed:
  • 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
    National Yang Ming Chiao Tung University)

  • 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)

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.

Suggested Citation

  • 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 , 2024. "Spin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-023-44469-4
    DOI: 10.1038/s41467-023-44469-4
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