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铁单体或氧化碳的铁单体:哪一个更适合电催化降解反应?

Rui Yang¹, Denglei Gao¹, Wei Li²

¹School of Chemical Engineering and Technology, Tianjin University, Tianjin 300354, P. R. China.

ACS applied materials & interfaces

|May 22, 2024

概括

与单原子催化剂 (SAC) 相比,原子催化剂 (ACC) 在电催化降解反应 (NRR) 中表现优越. 铁 (Fe3) 剪裁器比铁 (Fe1) 单体更有效地促进激活和氨合成.

科学领域:

电触媒溶解是一种电触媒.
材料科学材料科学材料科学
化学工程是化学工程的重要组成部分.

背景情况:

电催化降解反应 (NRR) 是哈伯-博什工艺的一个潜在替代方案.
单原子催化剂 (SAC) 对高效的NRR产生了兴趣,但它们对原子催化剂 (ACC) 的优势尚未完全确立.

研究的目的:

为了比较单原子催化剂 (Fe1) 与原子催化剂 (Fe3) 的NRR性能.
阐明Fe1和Fe3催化剂上的激活和还原的机制.

主要方法:

在添加碳支持上合成Fe单体 (Fe1) 和trimers (Fe3).
对NRR进行电催化性能测试.
密度函数理论 (DFT) 计算用于研究吸附和反应途径.

主要成果:

铁3催化剂显示出明显更高的氨产率 (27.89 μg h−1 mg−1_cat.) 与Fe1催化剂 (10.98μg h−1 mg−1_cat.%) 相比,Fe1催化剂的效率和法拉戴的效率为45.13%. 和20.98%的比例).
DFT计算显示,Fe3催化剂促进侧向吸附,并遵循具有较低NRR能量屏障的酶途径,与有利于端向吸附的Fe1催化剂不同.
对Fe3催化剂的增强N2激活归因于集群结构,促进侧向吸附.

结论:

原子催化剂,特别是Fe3,对于电催化NRR比单原子催化剂 (Fe1) 更有效.
在Fe3集群上N2的侧向吸附是增强催化活性的关键.
这项研究提供了设计优质NRR电催化剂的见解,通过偏好原子集群而不是单个原子.

关键词:

铁集群是指铁的集群.在 N2 激活过程中,N2 激活电催化降低的电催化剂酵素机制是一种酶机制.侧面吸附吸附方式

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