Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control

Wu, Jerry J.; Ji, Weijie; Au, Chak Tong

doi:10.1002/cctc.201701958

Cited by 29 publications

(20 citation statements)

References 291 publications

(269 reference statements)

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“…11−13 On the other hand, the rapid development in synthetic chemistry of high-surface area nanomaterials of well-defined surface and interface structures during the past two decades has established a useful nanomaterial database for us to specifically engineer the surface and interface parameters of heterogeneous metal catalysts with nearly atomic precision. 14,15 Such a capability allows us to fabricate model metal catalysts to avoid the interplay of different structural parameters for understanding the key factors that determine catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

Insights into the Interfacial Effects in Heterogeneous Metal Nanocatalysts toward Selective Hydrogenation

2021

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Heterogeneous metal catalysts are distinguished by their structure inhomogeneity and complexity. The chameleonic nature of heterogeneous metal catalysts have prevented us from deeply understanding their catalytic mechanisms at the molecular level and thus developing industrial catalysts with perfect catalytic selectivity toward desired products. This Perspective aims to summarize recent research advances in deciphering complicated interfacial effects in heterogeneous hydrogenation metal nanocatalysts toward the design of practical heterogeneous catalysts with clear catalytic mechanism and thus nearly perfect selectivity. The molecular insights on how the three key components (i.e., catalytic metal, support, and ligand modifier) of a heterogeneous metal nanocatalyst induce effective interfaces determining the hydrogenation activity and selectivity are provided. The interfaces influence not only the H2 activation pathway but also the interaction of substrates to be hydrogenated with catalytic metal surface and thus the hydrogen transfer process. As for alloy nanocatalysts, together with the electronic and geometric ensemble effects, spillover hydrogenation occurring on catalytically “inert” metal by utilizing hydrogen atom spillover from active metal is highlighted. The metal–support interface effects are then discussed with emphasis on the molecular involvement of ligands located at the metal–support interface as well as cationic species from the support in hydrogenation. The mechanisms of how organic modifiers, with the ability to induce both 3D steric and electronic effects, on metal nanocatalysts manipulate the hydrogenation pathways are demonstrated. A brief summary is finally provided together with a perspective on the development of enzyme-like heterogeneous hydrogenation metal catalysts.

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Section: Introductionmentioning

confidence: 99%

Insights into the Interfacial Effects in Heterogeneous Metal Nanocatalysts toward Selective Hydrogenation

2021

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“…[1−3] Since the hybridization effect strongly relies on the interfacial electronic coupling between hybridized species, [1] it is necessary to maximize this interfacial interaction to optimize the various functionalities of nanohybrids. [4] The unusually high surface-to-volume ratio of conductive two dimenstional (2D) nanosheets (NSs) renders these materials highly efficient hybridization matrices via effective interfacial interactions at their wide 2D surfaces. [5,6] To date, a huge number of reports have been published regarding the exploration of efficient energy-functional hybrid materials based on hybridization with conductive 2D NSs, such as reduced graphene oxide (rGO), 1T′-MoS 2 , RuO 2 , and MXene.…”

Section: Introductionmentioning

confidence: 99%

Multilayer Conductive Hybrid Nanosheets as Versatile Hybridization Matrices for Optimizing the Defect Structure, Structural Ordering, and Energy‐Functionality of Nanostructured Materials

Kwon

Kim

et al. 2021

Advanced Science

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The hybridization of conductive nanospecies has garnered significant research interest because of its high efficacy in improving the diverse functionalities of nanostructured materials. In this study, a novel synthetic strategy is developed to optimize the defect structure, structural ordering, and energy‐related functionality of nanostructured‐materials by employing a multilayer multicomponent two‐dimenstional (2D) graphene/metal oxide/graphene nanosheet (NS) as a versatile hybridization matrix. The hybridization of the robust trilayer, polydiallyldiammonium (PDDA)‐anchored reduced‐graphene oxide (prGO)/metal oxide/prGO NS effectively enhance the structural ordering and porosity of the hybridized MoS2/MnO2 NS through suppression of defect formation and tight stacking. In comparison with monolayer rGO/RuO2 NS‐based homologs, the 2D superlattice trilayer prGO/RuO2/prGO NS hybrids deliver better functionalities as a hydrogen evolution electrocatalyst and as a supercapacitor electrode, demonstrating the merits of hybridization with multilayer NSs. The advantages of using multilayer multicomponent conductive NSs as hybridization matrices arise from the enhancement of charge and mass transport through the layer flattening or defect suppression of the hybridized NSs and the increase in porosity, as evidenced by density functional theory calculations. Finally, the universal utility of multilayer NSs is confirmed by investigating the strong effect of the stacking order on the electrocatalytic functionality of MoS2/rGO/RuO2 films fabricated through layer‐by‐layer deposition.

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“…To enhance the activity of ceria‐based catalysts in PM oxidation, one critical factor to be considered is the morphology. The structural design at the nanoscale is critical in catalyst development . Since PM is a solid particle reactant, contact between PM and the catalyst strongly limits the reaction sites of PM oxidation .…”

Section: Introductionmentioning

confidence: 99%

“…The structural design at the nanoscale is critical in catalyst development. [8] Since PM is a solid particle reactant, contact between PM and the catalyst strongly limits the reaction sites of PM oxidation. [9] Accordingly, an increased number of contact points enhances the catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Ce‐Pr Mixed Oxide Catalysts with a Fibrous Morphology for Low‐temperature PM Oxidation

Jeong

Lee

et al. 2019

ChemCatChem

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Ceria (CeO2) is an effective precious‐metal‐free catalyst that combusts PM (particulate matter), due to its ability to switch between Ce4+ and Ce3+. In this work, to improve the activity of a ceria‐based catalyst, cerium‐praseodymium mixed oxide catalysts with various Ce−Pr ratios were synthesized with nanofiber morphologies, characterized, and compared with ceria catalysts. Two factors were considered: morphology and Ce−Pr ratio, which result in synergistic effects. In the ceria catalyst, we confirmed that a fibrous morphology is more advantageous for PM oxidation compared to nanocubes and nanorods with cubes, even though these samples have larger surface areas. In addition, the incorporation of Pr into the ceria nanofiber catalyst enhanced its intrinsic properties by promoting the reducibility and formation of oxygen vacancies. The analysis showed improved oxygen storage and supply capacity, especially for oxygen that is chemically adsorbed on the catalytic surface. PM oxidation tests demonstrated the Ce0.5Pr0.5O2‐NF catalyst showed the best activity in air, which was consistent with the characterization results. Thus, the Ce0.5Pr0.5O2‐NF sample was shown to be an effective and promising catalyst for PM oxidation.

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Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control

Cited by 29 publications

References 291 publications

Insights into the Interfacial Effects in Heterogeneous Metal Nanocatalysts toward Selective Hydrogenation

Insights into the Interfacial Effects in Heterogeneous Metal Nanocatalysts toward Selective Hydrogenation

Multilayer Conductive Hybrid Nanosheets as Versatile Hybridization Matrices for Optimizing the Defect Structure, Structural Ordering, and Energy‐Functionality of Nanostructured Materials

Ce‐Pr Mixed Oxide Catalysts with a Fibrous Morphology for Low‐temperature PM Oxidation

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