氢在单原子和Au负载的Pd和Pt小簇上顺序吸附的密度泛函计算(111)

IF 2.7 4区化学 Q3 CHEMISTRY, PHYSICAL

Electrocatalysis Pub Date : 2022-12-09 DOI:10.1007/s12678-022-00802-x

Joshua Meléndez-Rivera, Juan A. Santana

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引用次数: 0

摘要

我们利用密度泛函理论计算研究了氢在钯和铂原子位催化剂上的顺序吸附，如单原子合金催化剂(SAAC)、单原子催化剂(SAC)和单团簇催化剂(SCC)在Au(111)上的顺序吸附。结果表明，在不同的吸附氢覆盖条件下，Pd体系的氢吸附自由能趋于接近于零(\(\Delta {G}_{{\mathrm{H}}_{\mathrm{ads}}}\approx 0\))。在Pt体系的情况下，\(\Delta {G}_{{\mathrm{H}}_{\mathrm{ads}}}\approx 0\)仅在吸附氢的高覆盖条件下。这种差异来自于氢对Pd和Pt上的高配位和低配位的偏好。在Pt/Au的SCC中，氢的低配位导致\(\Delta {G}_{{\mathrm{H}}_{\mathrm{ads}}}\approx 0\)有多个吸附位点。这些结果有助于了解Pd/Au和Pt/Au的不同催化性能。图形摘要

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Density Functional Calculations of the Sequential Adsorption of Hydrogen on Single Atom and Small Clusters of Pd and Pt Supported on Au(111)

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Density Functional Calculations of the Sequential Adsorption of Hydrogen on Single Atom and Small Clusters of Pd and Pt Supported on Au(111)

We have used density functional theory calculations to study the sequential adsorption of hydrogen on Pd and Pt atomic site catalysts such as single-atom alloy catalysts (SAAC), single-atom catalysts (SAC), and single cluster catalysts (SCC) on Au(111). The results show that Pd systems tend to have near-zero free energy of hydrogen adsorption (\(\Delta {G}_{{\mathrm{H}}_{\mathrm{ads}}}\approx 0\)) under various coverage conditions of adsorbed hydrogen. In the case of Pt systems, \(\Delta {G}_{{\mathrm{H}}_{\mathrm{ads}}}\approx 0\) only at high coverage conditions of adsorbed hydrogen. Such differences come from the preference of hydrogen for high-coordination and low-coordination sites on Pd and Pt, respectively. The low coordination of hydrogen results in multiple adsorption sites with \(\Delta {G}_{{\mathrm{H}}_{\mathrm{ads}}}\approx 0\) in SCC of Pt/Au. These results can help to understand the different catalytic properties of Pd/Au and Pt/Au.

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来源期刊

Electrocatalysis CHEMISTRY, PHYSICAL-ELECTROCHEMISTRY

CiteScore

4.80

自引率

6.50%

发文量

审稿时长

>12 weeks

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