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  1. Article ; Online: Selective Benzyl Alcohol Oxidation over Pd Catalysts

    Carine Edith Chan-Thaw / Aditya Savara / Alberto Villa

    Catalysts, Vol 8, Iss 10, p

    2018  Volume 431

    Abstract: In the last decades, the selective liquid phase oxidation of alcohols to the corresponding carbonyl compounds has been a subject of growing interest. Research has focused on green methods that use “clean” oxidants such as O2 in combination with supported ...

    Abstract In the last decades, the selective liquid phase oxidation of alcohols to the corresponding carbonyl compounds has been a subject of growing interest. Research has focused on green methods that use “clean” oxidants such as O2 in combination with supported metal nanoparticles as the catalyst. Among the alcohols, benzyl alcohol is one of the most studied substrates. Indeed, benzyl alcohol can be converted to benzaldehyde, largely for use in the pharmaceutical and agricultural industries. This conversion serves as model reaction in testing new potential catalysts, that can then be applied to other systems. Pd based catalysts have been extensively studied as active catalytic metals for alcohol oxidation for their high activity and selectivity to the corresponding aldehyde. Several catalytic materials obtained by careful control of the morphology of Pd nanoparticles, (including bimetallic systems) and by tuning the support properties have been developed. Moreover, reaction conditions, including solvent, temperature, pressure and alcohol concentration have been investigated to tune the selectivity to the desired products. Different reaction mechanisms and microkinetic models have been proposed. The aim of this review is to provide a critical description of the recent advances on Pd catalyzed benzyl alcohol oxidation.
    Keywords palladium ; benzyl alcohol ; oxidation ; Chemical technology ; TP1-1185 ; Chemistry ; QD1-999
    Subject code 540 ; 660
    Language English
    Publishing date 2018-09-01T00:00:00Z
    Publisher MDPI AG
    Document type Article ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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  2. Article ; Online: Harnessing strong metal–support interactions via a reverse route

    Peiwen Wu / Shuai Tan / Jisue Moon / Zihao Yan / Victor Fung / Na Li / Shi-Ze Yang / Yongqiang Cheng / Carter W. Abney / Zili Wu / Aditya Savara / Ayyoub M. Momen / De-en Jiang / Dong Su / Huaming Li / Wenshuai Zhu / Sheng Dai / Huiyuan Zhu

    Nature Communications, Vol 11, Iss 1, Pp 1-

    2020  Volume 10

    Abstract: Strong metal–support interactions (SMSI) are effective in tuning the structures and catalytic performances of catalysts but limited by the poor exposure of active sites. Here, the authors develop a strategy to engineer SMSI via a reverse route, which is ... ...

    Abstract Strong metal–support interactions (SMSI) are effective in tuning the structures and catalytic performances of catalysts but limited by the poor exposure of active sites. Here, the authors develop a strategy to engineer SMSI via a reverse route, which is in favor of metal site exposure while embracing the SMSI.
    Keywords Science ; Q
    Language English
    Publishing date 2020-06-01T00:00:00Z
    Publisher Nature Portfolio
    Document type Article ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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  3. Article: Coupling of Acetaldehyde to Crotonaldehyde on CeO₂–ₓ(111): Bifunctional Mechanism and Role of Oxygen Vacancies

    Zhao, Chuanlin / Charles Watt / Paul R. Kent / Steven H. Overbury / David R. Mullins / Florencia C. Calaza / Aditya Savara / Ye Xu

    Journal of physical chemistry. 2018 Oct. 24, v. 123, no. 13

    2018  

    Abstract: Selective C–C coupling of oxygenates is pertinent to the manufacture of fuel and chemical products from biomass and from derivatives of C₁ compounds (i.e., oxygenates produced from methane and CO₂). Here we report a combined experimental and theoretical ... ...

    Abstract Selective C–C coupling of oxygenates is pertinent to the manufacture of fuel and chemical products from biomass and from derivatives of C₁ compounds (i.e., oxygenates produced from methane and CO₂). Here we report a combined experimental and theoretical study on the temperature-programmed reaction (TPR) of acetaldehyde (AcH) on a partially reduced CeO₂–ₓ(111) thin film surface. The experiments have been carried out under ultra-high-vacuum conditions without continuous gas exposure, allowing better isolation of active sites and reactive intermediates than in flow reaction conditions. AcH does not undergo aldol condensation in a typical TPR procedure, even though the enolate form of AcH (CH₂CHO) is readily produced on CeO₂–ₓ(111) with oxygen vacancies. We find however that a tailored “double-ramp” TPR procedure is able to successfully produce an aldol adduct, crotonaldehyde (CrA). Using density functional theory calculations and microkinetic modeling we explore several possible C–C coupling pathways. We conclude that the double-ramp procedure allows surface oxygen vacancy dimers, stabilized by adsorbate occupation, to form dynamically during the TPR. The vacancy dimers in turn enable C–C coupling to occur between an enolate and an adjacent AcH molecule via a bifunctional enolate–keto mechanism that is distinct from conventional acid- or base-catalyzed aldol condensation reactions. The proposed mechanism indicates that CrA desorption is rate-limiting while C–C coupling is facile.
    Keywords acetaldehyde ; active sites ; biomass ; carbon dioxide ; condensation reactions ; density functional theory ; desorption ; fuels ; manufacturing ; methane ; models ; oxygen
    Language English
    Dates of publication 2018-1024
    Size p. 8273-8286.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1932-7455
    DOI 10.1021/acs.jpcc.8b08535
    Database NAL-Catalogue (AGRICOLA)

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