Adhesion of Pt Nanoparticles Supported on γ-Al<sub>2</sub>O<sub>3</sub> Single Crystal

Zhang, Zhongfan; Li, Long; Yang, Judith C.

doi:10.1021/jp407798b

Cited by 17 publications

(18 citation statements)

References 57 publications

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“…Note that platinum has a weaker interfacial interaction with γ-Al 2 O 3 than with SrTiO 3 and the minimum energy Winterbottom shape of Pt on γ-Al 2 O 3 is closer to that of a free Wulff particle, facilitating the sintering. 39…”

Section: Results and Discussionmentioning

confidence: 99%

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Upcycling Single-Use Polyethylene into High-Quality Liquid Products

et al. 2019

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Our civilization relies on synthetic polymers for all aspects of modern life; yet, inefficient recycling and extremely slow environmental degradation of plastics are causing increasing concern about their widespread use. After a single use, many of these materials are currently treated as waste, underutilizing their inherent chemical and energy value. In this study, energy-rich polyethylene (PE) macromolecules are catalytically transformed into value-added products by hydrogenolysis using well-dispersed Pt nanoparticles (NPs) supported on SrTiO3 perovskite nanocuboids by atomic layer deposition. Pt/SrTiO3 completely converts PE (Mn = 8000–158,000 Da) or a single-use plastic bag (Mn = 31,000 Da) into high-quality liquid products, such as lubricants and waxes, characterized by a narrow distribution of oligomeric chains, at 170 psi H2 and 300 °C under solvent-free conditions for reaction durations up to 96 h. The binding of PE onto the catalyst surface contributes to the number averaged molecular weight (Mn) and the narrow polydispersity (Đ) of the final liquid product. Solid-state nuclear magnetic resonance of 13C-enriched PE adsorption studies and density functional theory computations suggest that PE adsorption is more favorable on Pt sites than that on the SrTiO3 support. Smaller Pt NPs with higher concentrations of undercoordinated Pt sites over-hydrogenolyzed PE to undesired light hydrocarbons.

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Section: Results and Discussionmentioning

confidence: 99%

“…The cube-on-cube epitaxy contributes to a large interfacial energy term for the Pt/SrTiO 3 interface, which in turn stabilizes the Pt NPs. 37−39…”

Section: Introductionmentioning

confidence: 99%

Upcycling Single-Use Polyethylene into High-Quality Liquid Products

et al. 2019

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“…For example, Pt/ alumina catalysts have no evidenceo fp referred Pt N orientation. [34][35][36] However,f or Pt/STO N ,P t N grow primarilyi nac ubeon-cube epitaxy on the (0 01)f acets of STO N . [1,31] We varied the composition from SrTiO 3 nanocuboids to BaTiO 3 nanocuboids (BTO N )t hat increased the substrate lattice parameter to introduce strain in Pt N .T his has the effect of increasing the interfacial energy between Pt N and the support as the Ba content is increased.…”

Section: Atomiclayer Depositionmethodology and Pt N /Ba X Sr 1àx Tio mentioning

confidence: 99%

“…Support–particle interactions can determine the relative orientation of the nanoparticle on the support. For example, Pt/alumina catalysts have no evidence of preferred Pt N orientation . However, for Pt/STO N , Pt N grow primarily in a cube‐on‐cube epitaxy on the (0 0 1) facets of STO N .…”

Section: Introductionmentioning

confidence: 99%

Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba_xSr_1−xTiO₃ Nanocuboids

et al. 2018

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The structure sensitivity of Pt nanoparticles (PtN) for gas‐phase acrolein (AC) hydrogenation was probed for PtN on BaxSr1−xTiO3 nanocuboid supports with (0 0 1) facets in a combined theoretical and experimental study. The in situ selectivity for allyl alcohol increased with the increase of the Sr concentration in the support, which corresponds to modifications in the stable Winterbottom shape and lattice strain of the Pt nanoparticles as a result of the interfacial energy between Pt and the BaxSr1−xTiO3 supports. “Local model” nanofacets of the Pt surface, edge, and corner morphologies were developed as compact representations of adsorption and reaction sites. DFT was used as the primary modeling tool for the equilibrium adsorption states. We argue that adsorption on edge sites is critically important for the overall allyl alcohol selectivity of PtN catalysts. A simple model was developed to represent PtN strain effects caused by its interaction with the substrate. Bader topological atom, spherical volume averaging charge, and modified bond valence sum analyses were used to understand the bonding structure. Density of states analysis was performed for the structures of PtN, adsorbed AC, and intermediate products to examine adsorbate–particle interactions. The simulated hydrogenation of AC on PtN nanofacets was compared to the in situ hydrogenation of AC by PtN on BaxSr1−xTiO3 to examine the effects of facet, edge, and corner sites on the overall selectivity.

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“…In addition, the NPs have to adhere strongly to the support in order to minimize the sintering of the particles at high temperatures. 28,29 In our method a proper mixing of the microemulsions, which contain metal NPs together with the support particles will increase the possibility of obtaining a homogeneous distribution of the particles on the support. During the deposition process, the adhesion of the metal NPs to the support material is dependent on the electrostatic interaction between the NPs and the support surface.…”

Section: Introductionmentioning

confidence: 99%

Support effect in the preparation of supported metal catalysts via microemulsion

et al. 2014

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It is well known that the activities of supported metal catalysts are strongly dependent upon the size, shape and dispersion of the nanoparticles on the support material. There are several techniques which can be implemented in order to produce such catalysts, e.g. wet impregnation, however the deposition of nanoparticles (NPs) on the support material without agglomeration still proves a challenge. This is particularly significant when attempting to maintain the size and shape of the particles during the deposition process. We have introduced a new method to deposit metal NPs, namely thermo-destabilization of microemulsions (please see J. Mater. Chem., 2012, 22, 11605–11614 and Nanoscale, 2013, 5, 796–805), in which the NPs are formed prior the deposition process. This method is an ingenious approach to control the dispersion of NPs on the support material and depositing NPs evenly with a narrow size distribution. In this paper we expound the important role of the surface charges of NPs and the support material, as indicated by zeta potentials, on the metal dispersion, and how they affect the catalytic activity. We also investigate the influence of other parameters such as the pore size and the pre-calcination of the support on the catalytic activities of the resulting supported metal catalysts.DFG, EXC 314, Unifying Concepts in Catalysi

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Adhesion of Pt Nanoparticles Supported on γ-Al₂O₃ Single Crystal

Cited by 17 publications

References 57 publications

Upcycling Single-Use Polyethylene into High-Quality Liquid Products

Upcycling Single-Use Polyethylene into High-Quality Liquid Products

Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba_xSr_1−xTiO₃ Nanocuboids

Support effect in the preparation of supported metal catalysts via microemulsion

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Adhesion of Pt Nanoparticles Supported on γ-Al2O3 Single Crystal

Cited by 17 publications

References 57 publications

Upcycling Single-Use Polyethylene into High-Quality Liquid Products

Upcycling Single-Use Polyethylene into High-Quality Liquid Products

Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on BaxSr1−xTiO3 Nanocuboids

Support effect in the preparation of supported metal catalysts via microemulsion

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Adhesion of Pt Nanoparticles Supported on γ-Al₂O₃ Single Crystal

Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba_xSr_1−xTiO₃ Nanocuboids