Enhancing the Catalytic Activity of Co Sites by the Synergistic Effect of Vacancy and Heterojunction Engineering for Efficient Electroreduction Nitrate to Ammonia

Enhancing the Catalytic Activity of Co Sites by the Synergistic Effect of Vacancy and Heterojunction Engineering for Efficient Electroreduction Nitrate to Ammonia Научная публикация

Журнал

Small
ISSN: 1613-6810 , E-ISSN: 1613-6829

Вых. Данные

Год: 2026, Номер статьи : e12893, Страниц : 14 DOI: 10.1002/smll.202512893

Авторы

Pan Yu ¹ , Xu Hui‐Min ¹ , Zhu Hong‐Rui ¹ , Lin Xue‐Shan ² , Song Lian‐Jie ³ , Lu Wan‐Qing ⁴ , Mao Jun ⁵ , Fominski Vyacheslav Yu. ⁶ , Maslov Mikhail M. ⁶ , Li Gao‐Ren ¹

Организации

1	College of Materials Science and Engineering Sichuan University Chengdu China
2	Chongqing Polytechnic University of Electronic Technology Chongqing China
3	China 19th Metallurgical Group Corporation Limited Chengdu China
4	Southwest Construction Co., Ltd. of CSCEC 7th Division Chongqing China
5	China Construction First Building (Group) Corporation Limited Beijing China
6	National Research Nuclear University MEPhI (Moscow Engineering Physics Institute) Moscow Russia

Electrocatalytic nitrate reduction reaction (NO3−RR) for ammonia synthesis is extremely compatible with the concept of green development as it enables both low carbon emission and low energy consumption ammonia (NH3) production, as well as the treatment of pollution in wastewater. However, the unavoidable competing reactions present in the NO3−RR process and adsorption limitations of the reactants on the surface hinder the effective activation of nitrate and affect the efficient NH3 synthesis. Herein, the high-performance VP- CoP/Co(OH)2 heterojunction catalysts for enhancing NO3−RR competition in the NO3− to NH3 conversion process was skillfully constructed by successfully growing Co(OH)2 nanosheets on P vacancy-rich CoP via an electrochemical in situ reconfiguration strategy. The optimized VP-CoP/Co(OH)2 exhibits excellent electrocatalytic performance of NO3−RR at −0.1 V vs. RHE, corresponding to an NH3 Faraday efficiency of 96.60% and an NH3 yield of 0.091 mmol h−1 cm−2, with a favorable stability. Combination of experimental studies and theoretical calculations demonstrates that P vacancies modify the coordination environment of the Co sites, which in turn modulates the electronic structure and accelerates the charge transfer rate. Heterojunctions, on the other hand, lead to a reconfiguration of the electronic structure at the interface, inducing a further accumulation of charge at the Co active sites. The synergy of both further activates the electronic states around the Co sites, which causes the d-band center moving toward the Fermi energy level, further enhancing the adsorption of NO3− and promoting the reduction of NO3−. This work focuses on modulating the electronic structure of the Co active sites to enhance its NO3−RR electrocatalytic performance, thus delivering a viable pathway for NO3− to NH3 high-efficiency conversion.

Pan Y. , Xu H. , Zhu H. , Lin X. , Song L. , Lu W. , Mao J. , Fominski V.Y. , Maslov M.M. , Li G.
Enhancing the Catalytic Activity of Co Sites by the Synergistic Effect of Vacancy and Heterojunction Engineering for Efficient Electroreduction Nitrate to Ammonia
Small. 2026. e12893 :1-14. DOI: 10.1002/smll.202512893 OpenAlex

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