Distribution of Pt single atom coordination environments on anatase TiO2 supports controls reactivity

Single-atom catalysts (SACs) offer efficient metal utilization and distinct reactivity compared to supported metal nanoparticles. Structure-function relationships for SACs often assume that active sites have uniform coordination environments at particular binding sites on support surfaces. Here, we...

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Published inNature communications Vol. 15; no. 1; p. 998
Main Authors Zang, Wenjie, Lee, Jaeha, Tieu, Peter, Yan, Xingxu, Graham, George W., Tran, Ich C., Wang, Peikui, Christopher, Phillip, Pan, Xiaoqing
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 02.02.2024
Nature Publishing Group
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Summary:Single-atom catalysts (SACs) offer efficient metal utilization and distinct reactivity compared to supported metal nanoparticles. Structure-function relationships for SACs often assume that active sites have uniform coordination environments at particular binding sites on support surfaces. Here, we investigate the distribution of coordination environments of Pt SAs dispersed on shape-controlled anatase TiO 2 supports specifically exposing (001) and (101) surfaces. Pt SAs on (101) are found on the surface, consistent with existing structural models, whereas those on (001) are beneath the surface after calcination. Pt SAs under (001) surfaces exhibit lower reactivity for CO oxidation than those on (101) surfaces due to their limited accessibility to gas phase species. Pt SAs deposited on commercial-TiO 2 are found both at the surface and in the bulk, posing challenges to structure-function relationship development. This study highlights heterogeneity in SA coordination environments on oxide supports, emphasizing a previously overlooked consideration in the design of SACs. Elucidating structure-function relationships is crucial for developing efficient catalysts. Here, the authors elucidate Pt single atom coordination environments on anatase TiO 2 and correlate active site structure with CO oxidation activity.
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ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-024-45367-z