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Spin Manipulation of Co sites in Co9S8/Nb2CTx Mott-Schottky Heterojunction for Boosting the Electrocatalytic Nitrogen Reduction Reaction.
Zhang, Shuai; Zhao, Weihua; Liu, Jiameng; Tao, Zheng; Zhang, Yinpeng; Zhao, Shuangrun; Zhang, Zhihong; Du, Miao.
Afiliación
  • Zhang S; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
  • Zhao W; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
  • Liu J; School of Medical Engineering, Xinxiang Medical University, Xinxiang, 453003, P. R. China.
  • Tao Z; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
  • Zhang Y; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
  • Zhao S; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
  • Zhang Z; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
  • Du M; College of Material and Chemical Engineering, Institute of New Energy Science and Technology, School of Future Hydrogen Energy Technology, Zhengzhou University of Light Industry, Zhengzhou, 450001, P. R. China.
Adv Sci (Weinh) ; : e2407301, 2024 Sep 03.
Article en En | MEDLINE | ID: mdl-39225309
ABSTRACT
Regulating the adsorption of an intermediate on an electrocatalyst by manipulating the electron spin state of the transition metal is of great significance for promoting the activation of inert nitrogen molecules (N2) during the electrocatalytic nitrogen reduction reaction (eNRR). However, achieving this remains challenging. Herein, a novel 2D/2D Mott-Schottky heterojunction, Co9S8/Nb2CTx-P, is developed as an eNRR catalyst. This is achieved through the in situ growth of cobalt sulfide (Co9S8) nanosheets over a Nb2CTx MXene using a solution plasma modification method. Transformation of the Co spin state from low (t2g 6eg 1) to high (t2g 5eg 2) is achieved by adjusting the interface electronic structure and sulfur vacancy of Co9S8/Nb2CTx-P. The adsorption ability of N2 is optimized through high spin Co(II) with more unpaired electrons, significantly accelerating the *N2→*NNH kinetic process. The Co9S8/Nb2CTx-P exhibits a high NH3 yield of 62.62 µg h-1 mgcat. -1 and a Faradaic efficiency (FE) of 30.33% at -0.40 V versus the reversible hydrogen electrode (RHE) in 0.1 m HCl. Additionally, it achieves an NH3 yield of 41.47 µg h-1 mgcat. -1 and FE of 23.19% at -0.60 V versus RHE in 0.1 m Na2SO4. This work demonstrates a promising strategy for constructing heterojunction electrocatalysts for efficient eNRR.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Sci (Weinh) Año: 2024 Tipo del documento: Article Pais de publicación: Alemania

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Sci (Weinh) Año: 2024 Tipo del documento: Article Pais de publicación: Alemania