Non-linear spin correlation of intermediates in enhanced electrochemical nitrate reduction under magnetic fields

Dongsheng Shao; Qian Wu; Yuwei Zhang; Xiyang Cai; Chencheng Dai; Siyuan Zhu; Fanxu Meng; Pengfei Song; Xiaoning Li; Xiaoming Ren; Tianze Wu; Zhichuan J. Xu

doi:10.1039/d5ee02132d

Non-linear spin correlation of intermediates in enhanced electrochemical nitrate reduction under magnetic fields

Dongsheng Shao, Qian Wu, Yuwei Zhang, Xiyang Cai, Chencheng Dai, Siyuan Zhu, Fanxu Meng, Pengfei Song, Xiaoning Li, Xiaoming Ren, Tianze Wu^*, Zhichuan J. Xu^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

Spin in electrocatalysis introduces a pivotal degree of freedom for overcoming thermodynamic and kinetic limitations. Paradigm studies on spin-related enhancement in oxygen electrocatalysis have highlighted the potential role of spin in influencing reaction kinetics. However, establishing spin correlations in reactions involving complex catalytic conversions, such as NH₃ synthesis, remains a significant challenge. Herein, we reveal spin correlations in electrochemical nitrate reduction (NO₃⁻RR) by demonstrating enhanced activity under external magnetic fields. The yield rate enhancement under magnetic fields is demonstrated on magnetic CuFe₂O₄ at 93.2% for NH₃ production and more than one order of magnitude for NO₂⁻ production. Linear and non-linear correlations between the activity enhancement and spin polarization improvement of CuFe₂O₄ are revealed for NO₃⁻RR toward NO₂⁻ and NH₃, respectively. Insights into spin polarization are provided on intermediates with different net spins, which facilitates the development of magnetic electrocatalysts for NO₃⁻RR.

Original language	English
Pages (from-to)	7708-7719
Number of pages	12
Journal	Energy and Environmental Science
Volume	18
Issue number	15
DOIs	https://doi.org/10.1039/d5ee02132d
Publication status	Published - Jul 29 2025
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2025 The Royal Society of Chemistry.

ASJC Scopus Subject Areas

Environmental Chemistry
Renewable Energy, Sustainability and the Environment
Nuclear Energy and Engineering
Pollution

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1039/d5ee02132d

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title = "Non-linear spin correlation of intermediates in enhanced electrochemical nitrate reduction under magnetic fields",

abstract = "Spin in electrocatalysis introduces a pivotal degree of freedom for overcoming thermodynamic and kinetic limitations. Paradigm studies on spin-related enhancement in oxygen electrocatalysis have highlighted the potential role of spin in influencing reaction kinetics. However, establishing spin correlations in reactions involving complex catalytic conversions, such as NH3 synthesis, remains a significant challenge. Herein, we reveal spin correlations in electrochemical nitrate reduction (NO3−RR) by demonstrating enhanced activity under external magnetic fields. The yield rate enhancement under magnetic fields is demonstrated on magnetic CuFe2O4 at 93.2\% for NH3 production and more than one order of magnitude for NO2− production. Linear and non-linear correlations between the activity enhancement and spin polarization improvement of CuFe2O4 are revealed for NO3−RR toward NO2− and NH3, respectively. Insights into spin polarization are provided on intermediates with different net spins, which facilitates the development of magnetic electrocatalysts for NO3−RR.",

author = "Dongsheng Shao and Qian Wu and Yuwei Zhang and Xiyang Cai and Chencheng Dai and Siyuan Zhu and Fanxu Meng and Pengfei Song and Xiaoning Li and Xiaoming Ren and Tianze Wu and Xu, \{Zhichuan J.\}",

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doi = "10.1039/d5ee02132d",

language = "English",

volume = "18",

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T1 - Non-linear spin correlation of intermediates in enhanced electrochemical nitrate reduction under magnetic fields

AU - Shao, Dongsheng

AU - Wu, Qian

AU - Zhang, Yuwei

AU - Cai, Xiyang

AU - Dai, Chencheng

AU - Zhu, Siyuan

AU - Meng, Fanxu

AU - Song, Pengfei

AU - Li, Xiaoning

AU - Ren, Xiaoming

AU - Wu, Tianze

AU - Xu, Zhichuan J.

PY - 2025/7/29

Y1 - 2025/7/29

N2 - Spin in electrocatalysis introduces a pivotal degree of freedom for overcoming thermodynamic and kinetic limitations. Paradigm studies on spin-related enhancement in oxygen electrocatalysis have highlighted the potential role of spin in influencing reaction kinetics. However, establishing spin correlations in reactions involving complex catalytic conversions, such as NH3 synthesis, remains a significant challenge. Herein, we reveal spin correlations in electrochemical nitrate reduction (NO3−RR) by demonstrating enhanced activity under external magnetic fields. The yield rate enhancement under magnetic fields is demonstrated on magnetic CuFe2O4 at 93.2% for NH3 production and more than one order of magnitude for NO2− production. Linear and non-linear correlations between the activity enhancement and spin polarization improvement of CuFe2O4 are revealed for NO3−RR toward NO2− and NH3, respectively. Insights into spin polarization are provided on intermediates with different net spins, which facilitates the development of magnetic electrocatalysts for NO3−RR.

AB - Spin in electrocatalysis introduces a pivotal degree of freedom for overcoming thermodynamic and kinetic limitations. Paradigm studies on spin-related enhancement in oxygen electrocatalysis have highlighted the potential role of spin in influencing reaction kinetics. However, establishing spin correlations in reactions involving complex catalytic conversions, such as NH3 synthesis, remains a significant challenge. Herein, we reveal spin correlations in electrochemical nitrate reduction (NO3−RR) by demonstrating enhanced activity under external magnetic fields. The yield rate enhancement under magnetic fields is demonstrated on magnetic CuFe2O4 at 93.2% for NH3 production and more than one order of magnitude for NO2− production. Linear and non-linear correlations between the activity enhancement and spin polarization improvement of CuFe2O4 are revealed for NO3−RR toward NO2− and NH3, respectively. Insights into spin polarization are provided on intermediates with different net spins, which facilitates the development of magnetic electrocatalysts for NO3−RR.

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U2 - 10.1039/d5ee02132d

DO - 10.1039/d5ee02132d

M3 - Article

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SN - 1754-5692

VL - 18

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EP - 7719

JO - Energy and Environmental Science

JF - Energy and Environmental Science

IS - 15

ER -

Non-linear spin correlation of intermediates in enhanced electrochemical nitrate reduction under magnetic fields

Abstract

Bibliographical note

ASJC Scopus Subject Areas

UN SDGs

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