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单站点催化剂促进剂加速金属催化的硝基芳烃氢化。

Single-site catalyst promoters accelerate metal-catalyzed nitroarene hydrogenation.

机构信息

Key Laboratory of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou, 310028, China.

Department of Materials Science and Engineering, University of California, Davis, CA, 95616, United States.

出版信息

Nat Commun. 2018 Apr 10;9(1):1362. doi: 10.1038/s41467-018-03810-y.

DOI:10.1038/s41467-018-03810-y
PMID:29636468
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5893533/
Abstract

Atomically dispersed supported metal catalysts are drawing wide attention because of the opportunities they offer for new catalytic properties combined with efficient use of the metals. We extend this class of materials to catalysts that incorporate atomically dispersed metal atoms as promoters. The catalysts are used for the challenging nitroarene hydrogenation and found to have both high activity and selectivity. The promoters are single-site Sn on TiO supports that incorporate metal nanoparticle catalysts. Represented as M/Sn-TiO (M = Au, Ru, Pt, Ni), these catalysts decidedly outperform the unpromoted supported metals, even for hydrogenation of nitroarenes substituted with various reducible groups. The high activity and selectivity of these catalysts result from the creation of oxygen vacancies on the TiO surface by single-site Sn, which leads to efficient, selective activation of the nitro group coupled with a reaction involving hydrogen atoms activated on metal nanoparticles.

摘要

原子分散负载型金属催化剂由于兼具新型催化性能和金属的高效利用而受到广泛关注。我们将这一类材料扩展到包含原子分散金属原子作为促进剂的催化剂中。这些催化剂用于具有挑战性的硝基芳烃加氢反应,并表现出高活性和选择性。促进剂是负载在 TiO 上的单原子 Sn,它包含金属纳米颗粒催化剂。这些催化剂表示为 M/Sn-TiO(M = Au、Ru、Pt、Ni),与未促进的负载金属相比,即使对于带有各种可还原基团的硝基芳烃加氢,它们也表现出更高的活性和选择性。这些催化剂的高活性和选择性源于单原子 Sn 在 TiO 表面上形成氧空位,这导致硝基基团的有效、选择性活化,同时涉及金属纳米颗粒上的氢原子的反应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/9114584fc146/41467_2018_3810_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/9a7372ba65b2/41467_2018_3810_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/b270449e9ef5/41467_2018_3810_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/9114584fc146/41467_2018_3810_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/9a7372ba65b2/41467_2018_3810_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/b270449e9ef5/41467_2018_3810_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/177c/5893533/9114584fc146/41467_2018_3810_Fig3_HTML.jpg

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