Yang Chen, Chen Yuanyuan, He Zhimin, Li Rong, Gou Xinglong
Precise Synthesis and Function Development Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering, China West Normal University, Nanchong, China.
Sichuan University of Arts and Science, Dazhou, China.
Front Chem. 2025 Jul 17;13:1629904. doi: 10.3389/fchem.2025.1629904. eCollection 2025.
The electrochemical nitrate reduction reaction (NITRR) offers a sustainable route for ammonia synthesis and environmental remediation but faces challenges such as sluggish kinetics and competing hydrogen evolution. This study aims to address these limitations by designing a Cu/molybdenum phosphide (MoP) heterostructure catalyst through one-pot calcination, which integrates Cu nanoparticles with MoP nanograins. Structural and electronic analyses confirm the formation of intimate Cu-MoP interfaces, where charge redistribution polarizes Cu to an electron-deficient state (Cu) and enriches MoP with electrons. This configuration enhances nitrate adsorption on Cu, while MoP efficiently supplies protons via accelerated water dissociation. The Cu/MoP catalyst achieves a record-high NH Faradaic efficiency (FE) of 98.93% and a yield rate of 30.72 mmol h cm at -0.5 V (vs. RHE), outperforming isolated Cu or MoP. When deployed in a Zn-nitrate battery, the composite cathode delivers a peak power density of 12.97 mW cm. This work provides a promising solution to the insufficient active hydrogen supply and poor NH conversion efficiency of Cu-based nitrate reduction catalysts.
电化学硝酸盐还原反应（NITRR）为氨合成和环境修复提供了一条可持续的途径，但面临着动力学缓慢和竞争性析氢等挑战。本研究旨在通过一锅煅烧设计一种铜/磷化钼（MoP）异质结构催化剂来解决这些限制，该催化剂将铜纳米颗粒与MoP纳米颗粒结合在一起。结构和电子分析证实了紧密的Cu-MoP界面的形成，其中电荷重新分布使铜极化到缺电子状态（Cuδ+）并使MoP富含电子。这种结构增强了硝酸盐在铜上的吸附，而MoP通过加速水离解有效地提供质子。Cu/MoP催化剂在-0.5 V（相对于可逆氢电极）下实现了创纪录的高NH3法拉第效率（FE）98.93%和产率30.72 mmol h-1 cm-2，优于单独的铜或MoP。当应用于硝酸锌电池时，复合阴极的峰值功率密度为12.97 mW cm-2。这项工作为铜基硝酸盐还原催化剂活性氢供应不足和NH3转化效率低的问题提供了一个有前景的解决方案。
