可逆氢电极
材料科学
异质结
法拉第效率
电催化剂
催化作用
钴
电化学
结晶学
电极
化学
物理化学
工作电极
光电子学
生物化学
冶金
作者
Shuai Zhang,Weihua Zhao,Jiameng Liu,Zheng Tao,Yinpeng Zhang,Shuangrun Zhao,Zhihong Zhang,Miao Du
标识
DOI:10.1002/advs.202407301
摘要
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 (N 2 ) during the electrocatalytic nitrogen reduction reaction (eNRR). However, achieving this remains challenging. Herein, a novel 2D/2D Mott–Schottky heterojunction, Co 9 S 8 /Nb 2 CT x ‐P, is developed as an eNRR catalyst. This is achieved through the in situ growth of cobalt sulfide (Co 9 S 8 ) nanosheets over a Nb 2 CT x MXene using a solution plasma modification method. Transformation of the Co spin state from low (t 2g 6 e g 1 ) to high (t 2g 5 e g 2 ) is achieved by adjusting the interface electronic structure and sulfur vacancy of Co 9 S 8 /Nb 2 CT x ‐P. The adsorption ability of N 2 is optimized through high spin Co(II) with more unpaired electrons, significantly accelerating the *N 2 →*NNH kinetic process. The Co 9 S 8 /Nb 2 CT x ‐P exhibits a high NH 3 yield of 62.62 µg h −1 mg cat. −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 NH 3 yield of 41.47 µg h −1 mg cat. −1 and FE of 23.19% at −0.60 V versus RHE in 0.1 m Na 2 SO 4 . This work demonstrates a promising strategy for constructing heterojunction electrocatalysts for efficient eNRR.
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