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铷铜合金纳米颗粒组成变化的电子结构演化。

Electronic Structure Evolution with Composition Alteration of RhCu Alloy Nanoparticles.

机构信息

Synchrotron X-ray Station at SPring-8, Research Network and Facility Services Division, National Institute for Materials Science (NIMS), 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan.

Synchrotron X-ray Group, Research Center for Advanced Measurement and Characterization, NIMS, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan.

出版信息

Sci Rep. 2017 Jan 25;7:41264. doi: 10.1038/srep41264.

DOI:10.1038/srep41264
PMID:28120907
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5264589/
Abstract

The change in electronic structure of extremely small RhCu alloy nanoparticles (NPs) with composition variation was investigated by core-level (CL) and valence-band (VB) hard X-ray photoelectron spectroscopy. A combination of CL and VB spectra analyses confirmed that intermetallic charge transfer occurs between Rh and Cu. This is an important compensation mechanism that helps to explain the relationship between the catalytic activity and composition of RhCu alloy NPs. For monometallic Rh and Rh-rich alloy (RhCu) NPs, the formation of Rh surface oxide with a non-integer oxidation state (Rh) resulted in high catalytic activity. Conversely, for alloy NPs with comparable Rh:Cu ratio (RhCu and RhCu), the decreased fraction of catalytically active Rh oxide is compensated by charge transfer from Cu to Rh. As a result, ensuring negligible change in the catalytic activities of the NPs with comparable Rh:Cu ratio to those of Rh-rich and monometallic Rh NPs.

摘要

采用芯能级（CL）和价带（VB）硬 X 射线光电子能谱研究了组成变化时极其微小的 RhCu 合金纳米粒子（NPs）的电子结构变化。CL 和 VB 谱分析的结合证实了 Rh 和 Cu 之间发生了金属间电荷转移。这是一种重要的补偿机制，有助于解释 RhCu 合金 NPs 催化活性与组成之间的关系。对于单金属 Rh 和 Rh 富合金（RhCu）NPs，形成具有非整数氧化态（Rh）的 Rh 表面氧化物导致高催化活性。相反，对于 Rh:Cu 比相当的合金 NPs（RhCu 和 RhCu），来自 Cu 到 Rh 的电荷转移补偿了催化活性 Rh 氧化物的减少。因此，确保了具有可比 Rh:Cu 比的 NPs 的催化活性与 Rh 富和单金属 Rh NPs 的催化活性几乎没有变化。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/96dbd15ae58f/srep41264-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/362b15837c61/srep41264-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/ba82dde5fa15/srep41264-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/4d07e902e645/srep41264-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/bb1904d0454d/srep41264-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/96dbd15ae58f/srep41264-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/362b15837c61/srep41264-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/ba82dde5fa15/srep41264-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/4d07e902e645/srep41264-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/bb1904d0454d/srep41264-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/abc9/5264589/96dbd15ae58f/srep41264-f5.jpg

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