Interfacial bonding stabilizes rhodium and rhodium oxide nanoparticles on layered Nb oxide and Ta oxide supports

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[1] Strayer, Megan E.
[2] Binz, Jason M.
[3] 3,Tanase, Mihaela
[4] Kamali Shahri, Seyed Mehdi
[5] Sharma, Renu
[6] Rioux, Robert M.
[7] Mallouk, Thomas E.
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Rioux, R.M. (rioux@engr.psu.edu) | 1600年 / American Chemical Society卷 / 136期
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Metal nanoparticles are commonly supported on metal oxides; but their utility as catalysts is limited by coarsening at high temperatures. Rhodium oxide and rhodium metal nanoparticles on niobate and tantalate supports are anomalously stable. To understand this; the nanoparticle-support interaction was studied by isothermal titration calorimetry (ITC); environmental transmission electron microscopy (ETEM); and synchrotron X-ray absorption and scattering techniques. Nanosheets derived from the layered oxides KCa2Nb 3O10; K4Nb6O17; and RbTaO3 were compared as supports to nanosheets of Na-TSM; a synthetic fluoromica (Na0.66Mg2.68(Si3.98Al 0.02)O10.02F1.96); and α-Zr(HPO 4)2·H2O. High surface area SiO 2 and γ-Al2O3 supports were also used for comparison in the ITC experiments. A Born-Haber cycle analysis of ITC data revealed an exothermic interaction between Rh(OH)3 nanoparticles and the layered niobate and tantalate supports; with H values in the range -32 kJ·mol-1 Rh to -37 kJ·mol-1 Rh. In contrast; the interaction enthalpy was positive with SiO2 and γ-Al2O3 supports. The strong interfacial bonding in the former case led to reverse ripening of micrometer-size Rh(OH)3; which dispersed as 0.5 to 2 nm particles on the niobate and tantalate supports. In contrast; particles grown on Na-TSM and α-Zr(HPO4)2·H2O nanosheets were larger and had a broad size distribution. ETEM; X-ray absorption spectroscopy; and pair distribution function analyses were used to study the growth of supported nanoparticles under oxidizing and reducing conditions; as well as the transformation from Rh(OH)3 to Rh nanoparticles. Interfacial covalent bonding; possibly strengthened by d-electron acid/base interactions; appear to stabilize Rh(OH)3; Rh2O3; and Rh nanoparticles on niobate and tantalate supports. © 2014 American Chemical Society;
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