光还原负载Ag优化Cu2O多面体电催化硝酸盐还原合成氨活性

doi:10.3976/j.issn.1002-4026.2025148

摘要/Abstract

摘要： 氨作为重要的化工原料，其传统合成工艺——哈伯-博施工艺存在高能耗、高排放等问题，因此开发绿色、高效的电催化合成氨技术具有重要意义。针对单一Cu₂O催化剂反应动力学迟滞以及电子转移速率较慢的问题，本文通过无模板化学沉淀法合成了26面体Cu₂O，并利用光还原法引入Ag颗粒负载于Cu₂O表面，降低催化剂阻抗，促进界面电荷传输，并增强了对*NO₂、*NH₂OH等反应中间体向NH₃转化的本征催化活性，抑制析氢反应和副产物生成，从而系统提升了电催化硝酸盐还原合成氨性能。电化学测试表明，Ag-Cu₂O在硝酸盐还原反应中表现出优异的催化性能，其氨法拉第效率最高达88%，优于Au-Cu₂O和纯Cu₂O，且副产物亚硝酸盐和竞争产物氢气生成量较少。该催化剂能够适应不同浓度NO₃^-溶液，为宽浓度范围硝酸盐废水处理提供帮助。本研究为设计高性能、高稳定性的硝酸盐还原电催化剂提供了新思路，对推动电催化技术在废水处理和绿色合成氨领域的应用具有参考价值。

关键词: 电催化, 硝酸根还原制氨, 光还原, 银, 氧化亚铜

Abstract: Ammonia is an important chemical feedstock. Its traditional synthesis process, Haber-Bosch process, suffers from issues such as high energy consumption and high emission. Therefore, it is of great significance to develop a green and efficient electrocatalytic ammonia synthesis technology. Aiming at the problems of sluggish reaction kinetics, slow electron transfer rate and easy reconstruction of single Cu2O, 26-faceted Cu2O polyhedral was synthesized by template-free chemical precipitation method, and Ag particles were loaded on the surface of Cu2O by photoreduction method. This approach optimized the electronic structure of the catalyst, promoted interfacial charge transfer, and enhanced the intrinsic catalytic activity for the conversion of key reaction intermediates (such as *NO2and *NH2OH) to NH3. Consequently, it inhibited the hydrogen evolution reaction and by-product formation, thereby improving the electrocatalytic nitrate reduction performance for ammonia synthesis. Electrochemical tests show that Ag-Cu2O exhibits excellent catalytic performance for the nitrate reduction reaction, and achieves a Faradaic efficiency of 88%, which is better than Au-Cu2O and pure Cu2O, while the generation of by-product nitrite and competitive product hydrogen are suppressed. The catalyst demonstrates adaptability to nitrate solutions of varying concentrations, offering potential for treating nitrate wastewater across a wide concentration range. This study provides a new strategy for designing high-performance and high-stability nitrate reduction electrocatalysts, and holds significant reference value for promoting the application of electrocatalytic technology in wastewater treatment and green ammonia synthesis.

Key words: electrocatalysis, nitrate reduction to ammonia, photoreduction, silver, copper oxide

中图分类号:

TQ113.247

程雅慧, 郭怡然, 温传敬. 光还原负载Ag优化Cu₂O多面体电催化硝酸盐还原合成氨活性[J]. 山东科学, 0, (): 1-.

CHENG Yahui, GUO Yiran, WEN Chuanjing. Photoreduction of Ag-loaded Cu2O polyhedra for optimizing the electrocatalytic activity of nitrate reduction to ammonia[J]. Shandong Science, 0, (): 1-.

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光还原负载Ag优化Cu₂O多面体电催化硝酸盐还原合成氨活性

Photoreduction of Ag-loaded Cu2O polyhedra for optimizing the electrocatalytic activity of nitrate reduction to ammonia

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