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Remote Activation Catalysis: Interparticle Hydrogen Spillover-Assisted Cumene Synthesis from Propane and Benzene.
Small
January 2025
Department of Chemistry and Life Science, Yokohama National University, Yokohama, 240-8501, Japan.
Hydrogen spillover, particularly when involving "interparticle" hydrogen spillover, offers a unique opportunity to enhance catalytic efficiency by remote activation of surface acidity. Building on this concept, this study aims to investigate physically mixed alumina-supported platinum nanoparticles (Pt/AlO) and zirconia-supported tungsten oxide (WO/ZrO) in promoting the direct synthesis of cumene from benzene and propane at 300 °C. The reaction with Pt/AlO alone afforded propylene as the only product, indicating the successive reaction route of Pt-catalyzed dehydrogenation of propane, followed by acid-catalyzed alkylation.
View Article and Find Full Text PDFSeparating nanobubble nucleation for transfer-resistance-free electrocatalysis.
Nat Commun
January 2025
School of Materials Science and Engineering, Nanyang Technological University, Singapore, Singapore.
Electrocatalytic gas-evolving reactions often result in bubble-covered surfaces, impeding the mass transfer to active sites. Such an issue will be worsened in practical high-current-density conditions and can cause sudden cell failure. Herein, we develop an on-chip microcell-based total-internal-reflection-fluorescence-microscopy to enable operando imaging of bubbles at sub-50 nm and dynamic probing of their nucleation during hydrogen evolution reaction.
View Article and Find Full Text PDFFrom FCC to BCC: Engineering Pd Nuclearity in the PdCu Catalyst to Enhance Ethylene Selectivity in Acetylene Hydrogenation.
Inorg Chem
January 2025
School of Materials Science and Engineering, Northeastern University, Shenyang 110819, China.
The ability to finely tune the nuclearity of active metal sites is critical for designing highly selective catalysts, especially for hydrogenation processes. In this work, we developed a novel PdCu catalyst with an ordered body-centered cubic (BCC) structure, enabling precise control over Pd nuclearity to optimize selectivity. Using a facile polyol synthesis method, we modulated the Pd coordination environment, reducing the Pd-Pd coordination number from 3 (disordered face-centered cubic, FCC) to 0 (ordered BCC), thereby achieving full isolation of Pd by the surrounding Cu atoms.
View Article and Find Full Text PDFMechanistic Understanding of Dissociated Hydrogen in Cu/CeO-Catalyzed Methanol Synthesis.
ACS Appl Mater Interfaces
January 2025
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, People's Republic of China.
The hydrogen dissociation and spillover mechanism on oxide-supported Cu catalysts play a pivotal role in the hydrogenation of carbon dioxide to methanol. This study investigates the hydrogen spillover mechanism on Cu/CeO catalysts using spectral characterization under high-pressure reaction conditions and density functional theory (DFT) simulations. The research confirms that the Cu sites serve as the initial dissociation points for the hydrogen molecules.
View Article and Find Full Text PDFUnveiling of Hydrogen Spillover Mechanisms on Tungsten Oxide Surfaces.
J Am Chem Soc
January 2025
Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
Hydrogen spillover is an important process in catalytic hydrogenation reactions, facilitating H activation and modulating surface chemistry of reducible oxide catalysts. This study focuses on the unveiling of platinum-induced hydrogen spillover on monoclinic tungsten trioxide (γ-WO), employing ambient pressure X-ray photoelectron spectroscopy, density functional theory calculations and microkinetic modeling to investigate the dynamic evolution of surface states at varied temperatures. At room temperature, hydrogen spillover results in the formation of W and hydrogen intermediates (hydroxyl species and adsorbed water), facilitated by Pt metal clusters.
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