On the Design of the Metal–Support Interface in Methanol Electrocatalytic Oxidation

IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2024-10-11 DOI:10.1021/acs.cgd.3c0146610.1021/acs.cgd.3c01466
Bartłomiej M. Szyja*,  and , Joanna Zasada, 
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Abstract

In this work, we present a theoretical investigation of the SrTiO3 perovskite-supported Pd catalyst in the methanol electro-oxidation reaction. In order to determine the metal–support interactions, we designed a system consisting of a Pd (100) double layer supported on one of the two possible terminations of the (100) perovskite surface. These terminations are characterized by different reducibilities of the layers directly interacting with the Pd bilayer and result in the difference in the stability of the surface-bound intermediates. Despite the fact that the Pd surface is identical in terms of geometry, we observed significant differences in the overpotential required for the reaction; in the case of TiO2 termination, the overpotential has been determined to be 0.68 V, while in the case of SrO termination, it amounts to as much as 1.35 V. We further investigate the charge transfers within the components of the system and the geometries of the intermediates to unravel the role of the electron structure on the overall efficiency of the process.

This work investigates a SrTiO3 perovskite-supported Pd catalyst for methanol electro-oxidation. A Pd (100) double layer is supported on two surface terminations (TiO2 and SrO), leading to different reaction overpotentials. Despite identical Pd geometry, TiO2 termination shows a lower overpotential compared to SrO. The study analyzes charge transfers and intermediate structures to understand the impact of the electronic structure on reaction efficiency.

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论甲醇电催化氧化中金属-支持物界面的设计
在这项研究中,我们对 SrTiO3 包晶支撑钯催化剂在甲醇电氧化反应中的应用进行了理论研究。为了确定金属与支撑物之间的相互作用,我们设计了一个由钯 (100) 双层组成的系统,该双层支撑在 (100) 包晶石表面两种可能的端点之一上。这些端点的特点是直接与钯双层相互作用的层的还原性不同,从而导致表面结合中间产物的稳定性不同。尽管钯表面的几何形状相同,但我们观察到反应所需的过电位存在显著差异;在 TiO2 端接的情况下,过电位被确定为 0.68 V,而在 SrO 端接的情况下,过电位高达 1.35 V。我们进一步研究了体系各组分内部的电荷转移以及中间产物的几何形状,以揭示电子结构对整个过程效率的作用。钯(100)双层被支撑在两个表面终端(TiO2 和 SrO)上,从而导致不同的反应过电位。尽管钯的几何形状相同,但二氧化钛终端的过电位低于氧化锰终端。研究分析了电荷转移和中间结构,以了解电子结构对反应效率的影响。
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来源期刊
CiteScore
7.20
自引率
4.30%
发文量
567
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