Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Matsubu, John C.; Zhang, Shuyi; DeRita, Leo; Marinković, Nebojša; Chen, Jingguang G.; Graham, George W.; Pan, Xiaoqing; Christopher, Phillip

doi:10.1038/nchem.2607

Cited by 717 publications

(712 citation statements)

References 52 publications

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“…For example, supports may directly influence the performance of supported metal species through strong metal-support interactions, [4][5][6] including metal cluster anchoring 7 and nanoparticle encapsulation, 8,9 as well as direct participation in reaction pathways. 10 Away from the active regions of the catalyst surface, the highly porous nature of typical catalyst supports also dictates mass transport properties through the existence of highly tortuous pore networks.…”

Section: Introductionmentioning

confidence: 99%

Exploring catalyst passivation with NMR relaxation

2017

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NMR relaxation has recently emerged as a novel and non-invasive tool for probing the surface dynamics of adsorbate molecules within liquid-saturated mesoporous catalysts. The elucidation of such dynamics is of particular relevance to the study and development of solvated green catalytic processes, such as the production of chemicals and fuels from bio-resources. In this paper we develop and implement a protocol using high field 1 H NMR spin-lattice relaxation as a probe of the reorientational dynamics of liquids imbibed within mesoporous oxide materials. The observed relaxation of liquids within mesoporous materials is highly sensitive to the adsorbed surface layer, giving insight into tumbling behaviour of spin-bearing chemical environments at the pore surface. As a prototypical example of relevance to liquid-phase catalytic systems, we examine the mobility of liquid methanol within a range of common catalyst supports. In particular, through the calculation and comparison of a suitable interaction parameter, we assess and quantify changes to these surface dynamics upon replacing surface hydroxyl groups with hydrophobic alkyl chains. Our results indicate that the molecular tumbling of adsorbed methanol is enhanced upon surface passivation due to the suppression of surface-adsorbate hydrogen bonding interactions, and tends towards that of the unrestricted bulk liquid. A complex analysis in which we account for the influence of changing pore structure and surface chemistry upon passivation is discussed. The results presented highlight the use of NMR spin-lattice relaxation measurements as a non-invasive probe of molecular dynamics at surfaces of interest to liquidphase heterogeneous catalysis.3

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Section: Introductionmentioning

confidence: 99%

Exploring catalyst passivation with NMR relaxation

2017

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“…[1][2][3][4][5][6][7] In particular, heterogeneous photocatalysis that couples light with chemical reactions is of paramount importance in chemistry and energy applications. [8][9][10][11][12][13][14][15][16] Plasmonic enhancement is currently a hot topic in catalysis-driven chemistry and photonic materials due to its important role as the main mediator bridging solar energy with other energy forms. For instance, the photocatalytic water splitting reaction used for biomimetic plant photosynthesis represents a promising solution to the growing demands for clean and sustainable energy.…”

Section: Introductionmentioning

confidence: 99%

Hot‐Electron‐Mediated Photochemical Reactions: Principles, Recent Advances, and Challenges

Kim

Lin

Son

et al. 2017

Advanced Optical Materials

167

116

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Hot electron chemistry has drawn tremendous attention from applications related to materials, energy, sensing, and catalysis. The plasmon‐induced generation of hot electrons and their transfer behavior are very important for understanding plasmonic‐enhanced applications and for achieving practically useful efficiency. From a plasmonic perspective, well‐designed plasmonic structures that can manipulate surface plasmons are able to enhance the efficiencies of hot electron‐based processes. This progress report summarizes the recent experimental and theoretical advances on the hot electron effect, emphasizing the crucial role of surface plasmons that are highly designable by using metal nanostructures. In particular, recent breakthroughs in the emerging fields of heterogeneous catalysis based on the hot electron effect are highlighted. Important design principles, mechanisms, and concepts, as well as challenges and perspectives, are illustrated and discussed.

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“…Therefore, such surface‐embedded Pt/CeO 2 hybrids are different from the conventional metal‐loaded‐on‐oxide structures reported before, where Pt NPs almost attached on top of a continuous oxide surface, even if similar S–S interfacial redox reaction was used 25, 26, 27. In addition, although SMSI effect may also induce partial decoration of oxide overlayers to metal NPs (e.g., Pt) through high‐temperature annealing in a reducing atmosphere, such process often coarsens metal NPs up to a large size 28, 29…”

Section: Resultsmentioning

confidence: 98%

Embedding Ultrafine and High‐Content Pt Nanoparticles at Ceria Surface for Enhanced Thermal Stability

Bian

et al. 2017

Advanced Science

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Ultrafine Pt nanoparticles loaded on ceria (CeO2) are promising nanostructured catalysts for many important reactions. However, such catalysts often suffer from thermal instability due to coarsening of Pt nanoparticles at elevated temperatures, especially for those with high Pt loading, which leads to severe deterioration of catalytic performances. Here, a facile strategy is developed to improve the thermal stability of ultrafine (1–2 nm)‐Pt/CeO2 catalysts with high Pt content (≈14 wt%) by partially embedding Pt nanoparticles at the surface of CeO2 through the redox reaction at the solid–solution interface. Ex situ heating studies demonstrate the significant increase in thermal stability of such embedded nanostructures compared to the conventional loaded catalysts. The microscopic pathways for interparticle coarsening of Pt embedded or loaded on CeO2 are further investigated by in situ electron microscopy at elevated temperatures. Their morphology and size evolution with heating temperature indicate that migration and coalescence of Pt nanoparticles are remarkably suppressed in the embedded structure up to about 450 °C, which may account for the improved thermal stability compared to the conventional loaded structure.

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Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Cited by 717 publications

References 52 publications

Exploring catalyst passivation with NMR relaxation

Exploring catalyst passivation with NMR relaxation

Hot‐Electron‐Mediated Photochemical Reactions: Principles, Recent Advances, and Challenges

Embedding Ultrafine and High‐Content Pt Nanoparticles at Ceria Surface for Enhanced Thermal Stability

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