Interfacial Bonding Stabilizes Rhodium and Rhodium Oxide Nanoparticles on Layered Nb Oxide and Ta Oxide Supports

Strayer, Megan E.; Binz, Jason; Tanase, M.; Shahri, Seyed Mehdi Kamali; Sharma, Renu; Rioux, Robert M.

doi:10.1021/ja412933k

Cited by 58 publications

(95 citation statements)

References 51 publications

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“…28 HCa 2 Nb 3 O 10 ·1.5 H 2 O was exfoliated into nanosheets of TBA 0.24 H 0.76 Ca 2 Nb 3 O 10 in excess aqueous TBA + OH − solutions as described previously. 26,29 …”

Section: Resultsmentioning

confidence: 99%

“…26,30,31 20 mmol L −1 aqueous solutions were made from the metal salts CoBr 2 , NiSO 4 ·6H 2 O, CuSO 4 , and AgNO 3 . Appropriate amounts of the metal aqueous solutions were added to 50.0 mL exfoliated nanosheets to achieve a metal mass fraction deposition of 0.05.…”

Section: Methodsmentioning

confidence: 99%

“…Measurements were conducted as previously reported. 26 Aqueous metal halide precursors (10 mmol L −1 to 15 mmol L −1 ) were injected from the syringe into solutions of TBA 0.24 H 0.76 Ca 2 Nb 3 O 10 nanosheets (0.1 mmol L −1 to 4 mmol L −1 ). The iridium monomer solution was injected as a 0.5 mmol L −1 solution.…”

Section: Methodsmentioning

confidence: 99%

“…26 These heats were also found to be strongly dependent on the oxide support composition. Stronger interfacial bonding was found to inhibit nanoparticle sintering in vacuum and under reducing atmospheres at elevated temperatures.…”

Section: Introductionmentioning

confidence: 90%

“…Conversely, the interfacial bonding to main group oxide supports, such as silica and alumina, is endothermic and particle growth on these oxides occurs at a much lower temperature. 26 …”

Section: Introductionmentioning

confidence: 99%

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Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support

Strayer¹,

Senftle

Winterstein

et al. 2015

J. Am. Chem. Soc.

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The interfacial interactions between late transition metal/metal oxide nanoparticles and oxide supports impact catalysts’ activity and stability. Here, we report the use of isothermal titration calorimetry (ITC), electron microscopy and density functional theory (DFT) to explore periodic trends in the heats of nanoparticle-support interactions for late transition metal and metal oxide nanoparticles on layered niobate and silicate supports. Data for Co(OH)2, hydroxyiridate-capped IrOx.nH2O, Ni(OH)2, CuO, and Ag2O nanoparticles were added to previously reported data for Rh(OH)3 grown on nanosheets of TBA0.24H0.76Ca2Nb3O10 and a layered silicate. ITC measurements showed stronger bonding energies in the order Ag < Cu ≈ Ni ≈ Co < Rh < Ir on the niobate support, as expected from trends in M-O bond energies. Nanoparticles with exothermic heats of interaction were stabilized against sintering as revealed by temperature resolved images recorded using transmission electron microscopy. In contrast, ITC measurements showed endothermic interactions of Cu, Ni, and Rh oxide/hydroxide nanoparticles with the silicate and poor resistance to sintering. These trends in interfacial energies were corroborated by DFT calculations using single-atom and four-atom cluster models of surface-bound metal/metal oxide nanoparticles. Density of states and charge density difference calculations reveal that strongly bonded metals (Rh, Ir) transfer d-electron density from the adsorbed cluster to niobium atoms in the support; this mixing is absent in weakly binding metals, such as Ag and Au, and in all metals on the layered silicate support. The large differences between the behavior of nanoparticles on niobate and silicate supports highlight the importance of d-orbital interactions between the nanoparticle and support in controlling the nanoparticles’ stability.

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“…28 HCa 2 Nb 3 O 10 ·1.5 H 2 O was exfoliated into nanosheets of TBA 0.24 H 0.76 Ca 2 Nb 3 O 10 in excess aqueous TBA + OH − solutions as described previously. 26,29 …”

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 90%

“…Conversely, the interfacial bonding to main group oxide supports, such as silica and alumina, is endothermic and particle growth on these oxides occurs at a much lower temperature. 26 …”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support

Strayer¹,

Senftle

Winterstein

et al. 2015

J. Am. Chem. Soc.

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New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts

et al. 2019

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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201901905. Supported metal nanoparticles are widely used as catalysts in the industrial production of chemicals, but still suffer from deactivation because of metal leaching and sintering at high temperature. In recent years, serious efforts have been devoted to developing new strategies for stabilizing metal nanoparticles. Recent developments for preparing sinter-resistant metalnanoparticle catalysts via strong metal-support interactions, encapsulation with oxide or carbon layers and within mesoporous materials, and fixation in zeolite crystals, are briefly summarized. Furthermore, the current challenges and future perspectives for the preparation of highly efficient and extraordinarily stable metal-nanoparticle-based catalysts, and suggestions regarding the mechanisms involved in sinter resistance, are proposed. Nanoparticle Catalysts

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Atomic‐Scale Structure Dynamics of Nanocrystals Revealed By In Situ and Environmental Transmission Electron Microscopy

Zhao

Zhu

et al. 2023

Advanced Materials

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Nanocrystals are of great importance in material sciences and industry. Engineering nanocrystals with desired structures and properties is no doubt one of the most important challenges in the field, which requires deep insight into atomic‐scale dynamics of nanocrystals during the process. The rapid developments of in situ transmission electron microscopy (TEM), especially environmental TEM, reveal insights into nanocrystals to digest. According to the considerable progress based on in situ electron microscopy, a comprehensive review on nanocrystal dynamics from three aspects: nucleation and growth, structure evolution, and dynamics in reaction conditions are given. In the nucleation and growth part, existing nucleation theories and growth pathways are organized based on liquid and gas–solid phases. In the structure evolution part, the focus is on in‐depth mechanistic understanding of the evolution, including defects, phase, and disorder/order transitions. In the part of dynamics in reaction conditions, solid–solid and gas–solid interfaces of nanocrystals in atmosphere are discussed and the structure–property relationship is correlated. Even though impressive progress is made, additional efforts are required to develop the integrated and operando TEM methodologies for unveiling nanocrystal dynamics with high spatial, energy, and temporal resolutions.

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Interfacial Bonding Stabilizes Rhodium and Rhodium Oxide Nanoparticles on Layered Nb Oxide and Ta Oxide Supports

Cited by 58 publications

References 51 publications

Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support

Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support

New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts

Atomic‐Scale Structure Dynamics of Nanocrystals Revealed By In Situ and Environmental Transmission Electron Microscopy

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