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Importance of Interfacial Band Structure between the Substrate and Mn3O4 Nanocatalysts during Electrochemical Water Oxidation
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-12-30 , DOI: 10.1021/acscatal.9b03831
Moo Young Lee 1 , Heonjin Ha 1 , Kang Hee Cho 1 , Hongmin Seo 1 , Sunghak Park 1 , Yoon Ho Lee 1 , Sung-Joo Kwon 2 , Tae-Woo Lee 1 , Ki Tae Nam 1
Affiliation  

The charge transport in the film-type electrocatalysts for the oxygen evolution reaction is a significant factor affecting the overall catalytic performance. For instance, transition metal oxide-based catalysts film has an optimum coating thickness due to the charge transport limitation. In this article, we investigated the charge transport behavior at the interface between the catalysts and the underlying substrate, which has been less investigated than the two other charge-transporting interfaces, that is, the catalysts surfaces and the inner catalysts film. We observed that Mn3O4 nanocatalysts exhibited different oxygen-evolving performances depending on the underlying substrate, and this activity trend was correlated with the work function of the substrate. We analyzed the work function dependency based on the energy band structure at the catalysts–substrate interface and determined that the substrates with low work functions formed high Schottky barriers, disturbing the interfacial charge transport. On the basis of this understanding, we demonstrated that the catalytic activity of Mn3O4 nanocatalysts film can be significantly enhanced using industrially important Ti substrates that have a thin buffering interlayer with the proper work function.

中文翻译:

电化学水氧化过程中基质与Mn 3 O 4纳米催化剂之间界面能带结构的重要性

在膜型电催化剂中用于氧释放反应的电荷传输是影响整体催化性能的重要因素。例如,由于电荷传输的限制,过渡金属氧化物基催化剂膜具有最佳的涂层厚度。在本文中,我们研究了催化剂与下面的底物之间的界面处的电荷传输行为,该行为比其他两个电荷传输界面(即催化剂表面和内部催化剂膜)的研究较少。我们观察到Mn 3 O 4纳米催化剂表现出不同的氧释放性能,这取决于下面的底物,并且该活性趋势与底物的功函数相关。我们基于催化剂-底物界面的能带结构分析了功函数依赖性,并确定了具有低功函数的底物形成了高肖特基势垒,从而干扰了界面电荷的传输。在此基础上,我们证明了使用具有重要缓冲功能且具有适当功函数的工业上重要的Ti基材,可以显着提高Mn 3 O 4纳米催化剂膜的催化活性。
更新日期:2019-12-30
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