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负载于钆掺杂二氧化铈上的原子分散铂的活性位点，具有改善的一氧化碳氧化低温性能。

Active sites of atomically dispersed Pt supported on Gd-doped ceria with improved low temperature performance for CO oxidation.

作者信息

Li Yuanyuan, Wang Haodong, Song Haohong, Rui Ning, Kottwitz Matthew, Senanayake Sanjaya D, Nuzzo Ralph G, Wu Zili, Jiang De-En, Frenkel Anatoly I

机构信息

Department of Materials Science and Chemical Engineering, Stony Brook University Stony Brook NY 11794 USA

Chemical Sciences Division, Oak Ridge National Laboratory Oak Ridge TN 37831 USA.

出版信息

Chem Sci. 2023 Oct 17;14(44):12582-12588. doi: 10.1039/d3sc03988a. eCollection 2023 Nov 15.

DOI:10.1039/d3sc03988a
PMID:38020390
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10646890/
Abstract

"Single - atom" catalysts (SACs) have been the focus of intense research, due to debates about their reactivity and challenges toward determining and designing "single - atom" (SA) sites. To address the challenge, in this work, we designed Pt SACs supported on Gd-doped ceria (Pt/CGO), which showed improved activity for CO oxidation compared to its counterpart, Pt/ceria. The enhanced activity of Pt/CGO was associated with a new Pt SA site which appeared only in the Pt/CGO catalyst under CO pretreatment at elevated temperatures. Combined X-ray and optical spectroscopies revealed that, at this site, Pt was found to be d-electron rich and bridged with Gd-induced defects an oxygen vacancy. As explained by density functional theory calculations, this site opened a new path a dicarbonyl intermediate for CO oxidation with a greatly reduced energy barrier. These results provide guidance for rationally improving the catalytic properties of SA sites for oxidation reactions.

摘要

“单原子”催化剂（SACs）一直是深入研究的焦点，这是由于围绕其反应活性存在争议，以及在确定和设计“单原子”（SA）位点方面面临挑战。为应对这一挑战，在本工作中，我们设计了负载在钆掺杂二氧化铈上的铂单原子催化剂（Pt/CGO），与对照物Pt/二氧化铈相比，其对一氧化碳氧化表现出更高的活性。Pt/CGO活性增强与一个新的铂单原子位点有关，该位点仅在高温一氧化碳预处理下的Pt/CGO催化剂中出现。结合X射线和光谱学研究表明，在这个位点，发现铂富含d电子，并与钆诱导的缺陷——一个氧空位相连。正如密度泛函理论计算所解释的，这个位点为一氧化碳氧化开辟了一条通往二羰基中间体的新路径，且能垒大幅降低。这些结果为合理改善单原子位点在氧化反应中的催化性能提供了指导。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/01676f558453/d3sc03988a-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/5f18dc48feb7/d3sc03988a-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/00272aa30698/d3sc03988a-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/c2178e834070/d3sc03988a-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/1258ce8efc32/d3sc03988a-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/01676f558453/d3sc03988a-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/5f18dc48feb7/d3sc03988a-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/00272aa30698/d3sc03988a-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/c2178e834070/d3sc03988a-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/1258ce8efc32/d3sc03988a-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0a/10646890/01676f558453/d3sc03988a-f5.jpg

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