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在酸性介质中减少氧气的单原子铁催化剂:颗粒大小控制和热激活

Hanguang Zhang¹, Sooyeon Hwang², Maoyu Wang³

¹Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York , Buffalo, New York 14260, United States.

Journal of the American Chemical Society

|September 14, 2017

概括

我们开发了一种新型的,地球上丰富的原子铁 (Fe) 催化剂,用于酸性介质中的氧降解反应 (ORR),为燃料电池提供一个有前途的替代品.

科学领域:

材料科学
电化学
催化剂

背景情况:

替换白金组金属 (PGM) 催化剂以土壤丰富的材料对于广泛采用质子交换膜燃料电池 (PEMFC) 来说至关重要.
在酸性介质中氧降解反应 (ORR) 是PEMFC性能和耐久性的关键挑战.

研究的目的:

在酸性介质中开发高性能,无PGM的原子铁 (Fe) 催化剂.
阐明来自石化模酸框架 (ZIFs) 的Fe催化剂的形成机制和活性位结构.

主要方法:

合成化学Fe-dopedZIF,然后进行一阶段的热激活,以创建嵌入在多孔碳中的原子Fe位点.
通过控制ZIF前体纳米晶体大小来调整催化剂颗粒大小 (20-1000 nm).
在高达1100°C的热激活过程中,ORR活动与化学键变化的相关性.

主要成果:

实现了具有可调节颗粒大小的高性能原子Fe催化剂,在50nm显示最佳ORR活性.
确定了与FeN4物种相关的800°C活性位点的临界形成温度 (Fe2+与pyridinic N结合).
最好的催化剂在0.5M H2SO4中表现出0.85V的半波电位,与Pt/C相比只有30mV的差距,并显示出更高的稳定性.

结论:

开发的原子Fe催化剂来源于Fe-doped ZIFs,作为一种在酸性介质中无PGM的ORR替代品,具有很大的前景.
精确控制催化剂大小和活性部位结构对于优化ORR性能至关重要.
这项工作为未来的PEMFC应用设计了高效和稳定的无PGM催化剂.

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相关概念视频

Catalysis

Catalysis

The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.