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Photohole-oxidation-assisted anchoring of ultra-small Ru clusters onto TiO2 with excellent catalytic activity and stability
C. M. Li; S. T. Zhang; B. S. Zhang; D. S. Su; S. He; Y. F. Zhao; J. Liu; F. Wang; M. Wei; D. G. Evans; X. Duan
2013
Source PublicationJournal of Materials Chemistry A
ISSN2050-7488
Volume1Issue:7Pages:2461-2467
AbstractUltra-small metal clusters with good activity and stability are of great significance for their practical applications in catalysis and materials science. Here we report a photohole-oxidation-assisted approach for anchoring ultra-small Ru clusters (similar to 1.5 nm) with an extremely high density (similar to 10(17) m(-2)) onto TiO2 support. The resulting clusters have good thermal stability and exhibit excellent long-term catalytic activity for the hydrogenation of CO2 to methane (methanation). The anchoring process involves the oxidation of Ru3+ in solution by photogenerated holes on the TiO2 surface to give tiny RuO2 species (<0.8 nm) immobilized on the surface, followed by a H-2 reduction step to produce Ru-0 clusters. Aberration-corrected high-resolution transmission electron microscopy (Cs-HRTEM) observations identify the Ru-Ru bond length contraction at the metal surface (relative to the interior of the particle) as well as bond length changes in the defect region at the metal-support interface. Density functional theory (DFT) calculations further demonstrate that the ultra-small Ru clusters are well stabilized and tightly anchored onto the TiO2 substrate via Ru-O covalent bonding in the defect region of the metal-support interface. The high-dispersion of ultra-small Ru clusters as well as the strong chemical bonding at the interface account for their surprisingly high catalytic reactivity and excellent thermal/reaction stability. This synthetic method may open up a new way to fabricate thermally stable ultra-small metal clusters for practical industrial applications in catalysis.
description.department[li, changming ; zhang, shitong ; he, shan ; zhao, yufei ; liu, jie ; wang, fei ; wei, min ; evans, david g. ; duan, xue] beijing univ chem technol, state key lab chem resource engn, beijing 100029, peoples r china. [zhang, bingsen ; su, dangsheng] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china. ; li, cm (reprint author), beijing univ chem technol, state key lab chem resource engn, beijing 100029, peoples r china. ; weimin@mail.buct.edu.cn
KeywordLayered Double Hydroxides Co Oxidation Gold Nanoparticles Surface Photodeposition Nanocomposites Particles Ag Nanostructures Semiconductor
URL查看原文
Language英语
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/71310
Collection中国科学院金属研究所
Recommended Citation
GB/T 7714
C. M. Li,S. T. Zhang,B. S. Zhang,et al. Photohole-oxidation-assisted anchoring of ultra-small Ru clusters onto TiO2 with excellent catalytic activity and stability[J]. Journal of Materials Chemistry A,2013,1(7):2461-2467.
APA C. M. Li.,S. T. Zhang.,B. S. Zhang.,D. S. Su.,S. He.,...&X. Duan.(2013).Photohole-oxidation-assisted anchoring of ultra-small Ru clusters onto TiO2 with excellent catalytic activity and stability.Journal of Materials Chemistry A,1(7),2461-2467.
MLA C. M. Li,et al."Photohole-oxidation-assisted anchoring of ultra-small Ru clusters onto TiO2 with excellent catalytic activity and stability".Journal of Materials Chemistry A 1.7(2013):2461-2467.
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