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通过CO吸附探测钯/铂合金纳米颗粒上的活性位点

Probing Active Sites on Pd/Pt Alloy Nanoparticles by CO Adsorption.

作者信息

Dolling Daniel Silvan, Chen Jiachen, Schober Jan-Christian, Creutzburg Marcus, Jeromin Arno, Vonk Vedran, Sharapa Dmitry I, Keller Thomas F, Plessow Philipp N, Noei Heshmat, Stierle Andreas

机构信息

Centre for X-ray and Nano Science CXNS, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.

Fachbereich Physik, Universität Hamburg, 20355 Hamburg, Germany.

出版信息

ACS Nano. 2024 Nov 12;18(45):31098-31108. doi: 10.1021/acsnano.4c08291. Epub 2024 Nov 2.

DOI:10.1021/acsnano.4c08291
PMID:39487797
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11562784/
Abstract

We studied the adsorption of CO on Pd/Pt nanoparticles (NPs) with varying compositions using polarization-dependent Fourier transform infrared reflection absorption spectroscopy (FT-IRRAS) and theoretical calculations (DFT). We prepared PtPd alloy NPs via physical vapor codeposition on α-AlO(0001) supports. Our morphological and structural characterization by scanning electron microscopy and grazing incidence X-ray diffraction revealed well-defined, epitaxial NPs. We used CO as a probe molecule to identify the particles' surface active sites. Polarization-dependent FT-IRRAS enabled us to distinguish CO adsorption on top and side facets of the NPs. The role of the Pd/Pt alloy ratio on CO adsorption was investigated by comparing the experimental CO stretching band frequency for different alloy arrangements to the results for pure Pd and Pt NPs. Moreover, we studied the influence of hydrogen adsorption on the NP surface composition. We determined the dependence of the IR bands on the local atomic arrangement via DFT calculations, revealing that both bulk alloy composition and neighboring atoms influence the wavenumber of the bands.

摘要

我们使用偏振相关傅里叶变换红外反射吸收光谱法（FT-IRRAS）和理论计算（DFT）研究了不同组成的钯/铂纳米颗粒（NPs）对一氧化碳的吸附情况。我们通过物理气相共沉积在α-AlO(0001)载体上制备了铂钯合金纳米颗粒。我们通过扫描电子显微镜和掠入射X射线衍射进行的形态和结构表征显示，纳米颗粒具有明确的外延结构。我们使用一氧化碳作为探针分子来识别颗粒的表面活性位点。偏振相关的FT-IRRAS使我们能够区分一氧化碳在纳米颗粒顶面和侧面的吸附。通过比较不同合金排列的实验一氧化碳伸缩带频率与纯钯和铂纳米颗粒的结果，研究了钯/铂合金比例对一氧化碳吸附的作用。此外，我们还研究了氢吸附对纳米颗粒表面组成的影响。我们通过DFT计算确定了红外波段对局部原子排列的依赖性，结果表明体相合金组成和相邻原子都会影响波段的波数。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/2b96cdef215e/nn4c08291_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/e92d50ba893a/nn4c08291_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/c2fa4d237add/nn4c08291_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/213e8b941fe1/nn4c08291_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/25503e6db92b/nn4c08291_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/878acbce53b8/nn4c08291_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/fe553b5809b8/nn4c08291_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/2b96cdef215e/nn4c08291_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/e92d50ba893a/nn4c08291_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/c2fa4d237add/nn4c08291_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/213e8b941fe1/nn4c08291_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/25503e6db92b/nn4c08291_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/878acbce53b8/nn4c08291_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/fe553b5809b8/nn4c08291_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/705e/11562784/2b96cdef215e/nn4c08291_0007.jpg

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本文引用的文献

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