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自动触发局部性微环境的Co₄Fe₆高效中性氨电合成

Yang Yang^1,2, Yuting Sun^1,3, Yuning Wang^1,4

¹Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang 110016, China.

Journal of the American Chemical Society

|February 28, 2025

概括

这项研究引入了Co4Fe6电催化剂,该电催化剂在中性水中有效地将酸盐 (NO3-) 转化为氨 (NH3). 这种突破避免了恶劣的环境和昂贵的金属,

科学领域:

电化学
材料科学
催化剂
环境化学

背景情况:

对于可持续的NH3合成和酸盐修复,电化学酸盐降解反应 (eNO3-RR) 对氨 (NH3) 是至关重要的.
目前基于Fe的电催化剂通常需要恶劣的性条件或贵金属才能在中性介质中有效地发挥作用.
基于pH的动力学和水分的限制阻碍了在中性电解质中开发高效的eNO3-RR电催化剂.

研究的目的:

开发一种高效的电催化剂,用于在中性介质中将酸盐降解为氨.
研究自我触发局部性的机制,以提高eNO3-RR活性.
展示基于Fe的合金在可持续酸盐上循环技术中的潜力.

主要方法:

Co4Fe6合金电催化剂的合成和特征.
在中性电解质中对eNO3-RR性能进行电化学评估.
现场/操作研究以了解反应机制和局部pH影响.
在膜电极组件 (MEA) 电解仪中进行长期稳定性测试.

主要成果:

Co4Fe6电催化剂的NH3法拉代效率 (FE) 高达98.6%,选择性为99.9%,比RHE低0.69V.
催化剂表现出自我触发的局部性,克服中性介质中的常规pH限制.
协同的 Co-Fe 双位点促进了最佳的反应途径和平衡的水分离与 NO2- 质子化.
在MEA中达到高电流密度 (100 mA cm-2),NH3 FE>96%和500小时以上的稳定性.

结论:

Co4Fe6电催化剂可以在中性介质中有效和选择性地将酸盐降解为氨.
自触发的局部性是提高Fe基合金eNO3-RR性能的一个关键因素.
这项工作为可持续的酸盐上循环提供了一个有希望的途径,而无需依赖性电解质或贵金属.

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