Catalysis is inherently driven by the interaction of reactants, intermediates and formed products with the catalyst’s surface. In order to reach the desired transition state and to overcome the kinetic barrier, elevated temperatures or electrical potentials are employed to increase the rate of reaction. Despite immense efforts in the last decades, research in thermo- and electrocatalysis has often preceded in isolation, even for similar reactions. Conceptually, any heterogeneous surface process that involves changes in oxidation states, redox processes, adsorption of charged species (even as spectators) or heterolytic cleavage of small molecules should be thought of as having parallels with electrochemical processes occurring at electrified interfaces. Herein, we compare current trends in thermo- and electrocatalysis and elaborate on the commonalities and differences between both research fields, with a specific focus on the production of hydrogen peroxide as case study. We hope that interlinking both fields will be inspiring and thought-provoking, eventually creating synergies and leverage towards more efficient decentralized chemical conversion processes.
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http://dx.doi.org/10.1038/s41467-022-29536-6 | DOI Listing |
Angew Chem Int Ed Engl
December 2024
Department of Chemistry, Tsinghua University, 100084, Beijing, China.
Selective electrocatalytic hydrogenation (ECH) of phenol is a sustainable route to produce cyclohexanone, an industrially important feedstock for polymer synthesis. However, attaining high selectivity and faradaic efficiency (FE) for cyclohexanone remain challenging, owning to over-hydrogenation of phenol to cyclohexanol and competition of hydrogen evolution reaction (HER). Herein, by employing hydrogen spillover effect, we modulate adsorbed hydrogen species (H) coverage on Pt surface via migration to TiO in an anatase TiO-supported Pt catalyst.
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October 2024
Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University Binhai New City, Fuzhou, 350207, China.
Traditional methods for the aerobic oxidation of methane to methanol frequently require the use of noble metal catalysts or flammable H-O mixtures. While electrochemical methods enhance safety and may avoid the use of noble metals, these processes suffer from low yields due to limited current density and/or low selectivity. Here, we design an electrothermal process to conduct aerobic oxidation of methane to methanol at room temperature using phosphotungstic acid (PTA) as a redox mediator.
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October 2024
Department of Materials Science and Engineering & Institute of Materials Science, University of Connecticut, 25 King Hill Road, Storrs, CT, 06269-3136, USA.
Hydrogen, as an important clean energy source, plays a more and more crucial role in decarbonizing the planet and meeting the global climate challenge due to its high energy density and zero-emission. The demand for sustainable hydrogen is increasing drastically worldwide as driven by the global shift towards low-carbon energy solutions. Thermochemical catalysis process dominates hydrogen production at scale given its relatively mature technology and commercialization status, as well as the established manufacturing infrastructure.
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January 2025
Department of Chemical Engineering, University of California, Santa Barbara, Santa Barbara, CA 93106-5080, United States.
Redox reactions on the surface of transition metal oxides are of broad interest in thermo, photo, and electrocatalysis. H temperature-programmed reduction (H-TPR) is commonly used to probe oxide reducibility by measuring the rate of H consumption during temperature ramps, assuming that this rate is controlled by oxide reduction. However, oxide reduction involves several elementary steps, such as H dissociation and H-spillover, before surface reduction and HO formation occur.
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September 2024
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, 1219 Zhongguan West Road, Ningbo, 315201, P.R. China.
2,5-Furandicarboxylic acid (FDCA) has emerged as an important bio-based furanic compound, which has broad application prospects in renewable energy and materials, especially in the preparation of polyethylene 2,5-furandicarboxylate (PEF). While the conventional synthesis of FDCA involves oxidation of 5-hydroxymethylfurfural (HMF) as a substitute, the thermal and chemical instability of HMF due to its aldehyde group poses challenges. A more favorable alternative is the utilization of 2,5-bis(hydroxymethyl)furan (BHMF), a non-aldehyde and more stable precursor.
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