Facet Engineering of a Metal–Organic Framework Support Modulates the Microenvironment of Palladium Nanoparticles for Selective Hydrogenation

Gao, Ming-Liang; Li, Luyan; Sun, Zi-Xuan; Li, Jiarui; Jiang, Hai‐Long

doi:10.1002/ange.202211216

Angewandte Chemie

2022

DOI: 10.1002/ange.202211216

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Facet Engineering of a Metal–Organic Framework Support Modulates the Microenvironment of Palladium Nanoparticles for Selective Hydrogenation

Ming-Liang Gao

Luyan Li

Zi-Xuan Sun

et al.

Abstract: The exposed facets of supported catalysts play a crucial role in catalysis; however, they are usually ignored and related studies remain rare. Herein, we have fabricated a series of sandwich-structured metalorganic framework composites, denoted ZIF-8 X @Pd@ZIF-8 (x represents the morphology of ZIF-8 core, i.e., ZIF-8 C exposing (100) facet, ZIF-8 RD exposing (110) facet, and ZIF-8 TRD exposing mixed ( 100) and (110) facets), featuring Pd nanoparticles deposited on the specific crystal facets of ZIF-8 core, for… Show more

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2024

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Cited by 3 publications

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Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H₂O in the Peroxidase‐Like Catalyzed Reaction

Shen,

Wu,

Guo

et al. 2024

Adv Funct Materials

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Hydrophilicity‐hydrophobicity modulation of active sites provides a promising strategy for enhancing catalytic performance. Current researches focus on the influence of substrate molecules, however, the role of H2O molecules is often overlooked in nanozyme‐catalyzed reactions. Herein, bioinspired Pt@ZIF‐R (R = ‐90, ‐8, ‐8@TMS, where TMS is tetraethoxysilane) nanozymes are designed as model catalysts, with Pt nanoparticles as active centers and metal organic‐framework nanocavities as hydrophilic‐hydrophobic binding pockets, revealing the critical role of H2O in the peroxidase‐like catalytic process of H2O2 decomposition. A positive correlation between catalytic activity and hydrophobicity is observed, and strong hydrophobic Pt@ZIF‐8@TMS nanozyme exhibits the best catalytic performance. Theoretical calculations indicate that as hydrophobicity increases, solvent H2O reduces the competitive adsorption with H2O2 and decreases the energy barrier of the rate‐determining step (2*O→*O2) simultaneously. In addition, the desorption of the product H2O is thermodynamically favorable with increasing hydrophobicity. Importantly, Pt@ZIF‐8@TMS nanozyme is successfully used to develop a colorimetric biosensor for the detection of organophosphorus pesticides, with a detection limit as low as 0.7 ng mL−1, which is superior to numerous existing methods. This work provides fundamental insights into the function of hydrophobicity in boosting catalytic activity, which may offer guidance for the development of efficient nanozymes.

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Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H₂O in the Peroxidase‐Like Catalyzed Reaction

Shen,

Wu,

Guo

et al. 2024

Adv Funct Materials

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Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO₂ to Methanol: Activity and Selectivity Insights

Velisoju,

Ramos‐Fernández,

Kancherla

et al. 2024

Angewandte Chemie

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Our study unveils a pioneering methodology that effectively distributes Pd species within a zeolitic imidazolate framework‐8 (ZIF‐8). We demonstrate that Pd can be encapsulated within ZIF‐8 as atomically dispersed Pd species that function as an excited‐state transition metal catalyst for promoting carbon–carbon (C–C) cross‐couplings at room temperature using visible light as the driving force. Furthermore, the same material can be reduced at 250 °C, forming Pd metal nanoparticles encapsulated in ZIF‐8. This catalyst shows high rates and selectivity for carbon dioxide hydrogenation to methanol under industrially relevant conditions (250 °C, 50 bar): 7.46 molmethanol molmetal−1 h−1 and >99%. Our results demonstrate the correlations of the catalyst structure with the performances at experimental and theoretical levels.

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Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO₂ to Methanol: Activity and Selectivity Insights

Velisoju,

Ramos‐Fernández,

Kancherla

et al. 2024

Angew Chem Int Ed

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Facet Engineering of a Metal–Organic Framework Support Modulates the Microenvironment of Palladium Nanoparticles for Selective Hydrogenation

Cited by 3 publications

References 63 publications

Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H₂O in the Peroxidase‐Like Catalyzed Reaction

Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H₂O in the Peroxidase‐Like Catalyzed Reaction

Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO₂ to Methanol: Activity and Selectivity Insights

Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO₂ to Methanol: Activity and Selectivity Insights

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Facet Engineering of a Metal–Organic Framework Support Modulates the Microenvironment of Palladium Nanoparticles for Selective Hydrogenation

Cited by 3 publications

References 63 publications

Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H2O in the Peroxidase‐Like Catalyzed Reaction

Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H2O in the Peroxidase‐Like Catalyzed Reaction

Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO2 to Methanol: Activity and Selectivity Insights

Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO2 to Methanol: Activity and Selectivity Insights

Contact Info

Product

Resources

About

Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H₂O in the Peroxidase‐Like Catalyzed Reaction

Modulating the Hydrophilic‐Hydrophobic Microenvironment of MOF‐Stabilized Pt Nanozymes: the Role of H₂O in the Peroxidase‐Like Catalyzed Reaction

Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO₂ to Methanol: Activity and Selectivity Insights

Highly Dispersed Pd@ZIF‐8 for Photo‐Assisted Cross‐Couplings and CO₂ to Methanol: Activity and Selectivity Insights