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在通用pH下有效的电催化降低的O诱导二原子Fe-Mo模拟酶

Yuanyuan Yu¹, Qingtong Zhang¹, Simin Wei¹

¹Guangxi Key Laboratory of Clean Pulp & Papermaking and Pollution Control, School of Light Industry and Food Engineering, Guangxi University, Nanning 530004, China.

Journal of the American Chemical Society

|July 28, 2025

概括

一种新的仿生催化剂通过电化学降解反应 (ENRR) 有效地合成氨. 这种Fe-Mo二原子催化剂在普遍pH下实现了创纪录的产量和稳定性.

科学领域:

电化学
催化剂
材料科学

背景情况:

电化学降解反应 (ENRR) 为氨合成提供了可持续的途径.
为ENRR设计高效的催化剂,特别是那些促进电子/质子转移和中间化的催化剂,仍然是一个重大挑战.

研究的目的:

设计一种由酶酶启发的仿生铁- (Fe-Mo) 二原子催化剂,用于增强ENRR.
调整催化剂的微环境,使用氧诱导的原子封闭效应来调节催化活性.

主要方法:

生物模拟Fe-Mo二原子催化剂 (FeMo-CDW ((CT-3h)) 的制造.
通过加入氧气调节催化剂的活性部位以产生原子封闭效应.
在通用pH值下进行电化学表征和氨产量测量.
理论计算 (DFT) 来阐明反应机制.

主要成果:

具有四个氧原子的FeMo-CDW ((CT-3h)) 催化剂在0.1M HCl中显示出336.03μg h−1 cm−2的破纪录的氨产量,超过之前的最大值三倍以上.
催化剂具有很高的稳定性,连续运行250小时,持续10个周期.
理论计算证实了因Fe-Mo d轨道与N2*混合而增强的电子转移,N键的减弱,以及加速的质子转移和化.

结论:

在Fe-Mo二原子催化剂中,O诱导的原子封闭效应对于优化ENRR中的电子和质子转移至关重要.
生物模拟FeMo-CDW ((CT-3h)) 催化剂代表了可持续氨合成的重大进步,提供了高效率和稳定性.
这项研究提供了用于电化学降低的先进催化剂设计的新策略.

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