数字农科院2.0

Metal complex-derived carbon-coated cobalt phosphide nanoparticles supported on C3N4 for efficient electrocatalytic nitrite reduction to ammonia

文献类型： 外文期刊

作者： Shenjie Liu;;Xin Zhao;;Jing Dong;;Chen Lei;;Chuanjun Wang;;Guoqiang Wang;;Jing Xu;;Wenbo Bai;;Geoffrey Waterhouse

关键词： Schiff base complexes;;Transition metal phosphides;;Carbon nitride;;Electrocatalytic ammonia synthesis;;Nitrite

期刊名称： Chemical Engineering Journal

ISSN： 1385-8947

年卷期： 2025 年

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： The electrochemical nitrite reduction reaction (eNO2RR) to ammonia (NH3) not only enables NO2−pollutant removal from water but also provides an alternative strategy for sustainable ammonia synthesis, making it a research hotspot in both water treatment and electrocatalysis in recent years. However, the complex reaction pathway of eNO2RR can lead to the generation of numerous byproducts, resulting in low Faradaic efficiency (FE) and poor selectivity to NH3. To address this, we fabricated a heterostructured composite electrocatalyst comprising carbon-encapsulated cobalt phosphide (CoP@C) nanoparticles supported on graphitic carbon nitride (C3N4) (denoted as CoP@C/C3N4) via a one-step low-temperature phosphidation method. This catalyst achieved an H3 production rate of 394.19 h−1cm−2 and a Faradaic efficiency of 91.17 % for the eNO2RR at −0.5 V (vs. RHE) under alkaline conditions. Notably, the CoP@C/C3N4 electrode also demonstrated excellent long-term stability, operating continuously for over 300 h under high current density conditions without significant degradation. The excellent electrocatalytic performance is attributable to synergistic effects between the C3N4 and the carbon encapsulation layer, which significantly enhances interfacial charge transfer kinetics, thereby boosting the catalytic efficiency. Furthermore, the two-dimensional (2D) sheet-like structure of C3N4 effectively anchors and uniformly disperses the CoP@C nanoparticles, while the carbon encapsulation layer suppresses loss of CoP active sites through a physical barrier effect. This work demonstrates a simple synthetic route and theoretical foundation for the development of highly efficient metal phosphide catalysts for lectrocatalytic nitrite-to-ammonia synthesis and other important electrocatalytic reactions.

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