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      Pt/ZrO 2 Prepared by Atomic Trapping: An Efficient Catalyst for the Conversion of Glycerol to Lactic Acid with Concomitant Transfer Hydrogenation of Cyclohexene

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          Abstract

          A series of heterogeneous catalysts consisting of highly dispersed Pt nanoparticles supported on nanosized ZrO 2 (20 to 60 nm) was synthesized and investigated for the one-pot transfer hydrogenation between glycerol and cyclohexene to produce lactic acid and cyclohexane, without any additional H 2. Different preparation methods were screened, by varying the calcination and reduction procedures with the purpose of optimizing the dispersion of Pt species (i.e., as single-atom sites or extra-fine Pt nanoparticles) on the ZrO 2 support. The Pt/ZrO 2 catalysts were characterized by means of transmission electron microscopy techniques (HAADF-STEM, TEM), elemental analysis (ICP-OES, EDX mapping), N 2-physisorption, H 2 temperature-programmed-reduction (H 2-TPR), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). Based on this combination of techniques it was possible to correlate the temperature of the calcination and reduction treatments with the nature of the Pt species. The best catalyst consisted of subnanometer Pt clusters (<1 nm) and atomically dispersed Pt (as Pt 2+ and Pt 4+) on the ZrO 2 support, which were converted into extra-fine Pt nanoparticles (average size = 1.4 nm) upon reduction. These nanoparticles acted as catalytic species for the transfer hydrogenation of glycerol with cyclohexene, which gave an unsurpassed 95% yield of lactic acid salt at 96% glycerol conversion (aqueous glycerol solution, NaOH as promoter, 160 °C, 4.5 h, at 20 bar N 2). This is the highest yield and selectivity of lactic acid (salt) reported in the literature so far. Reusability experiments showed a partial and gradual loss of activity of the Pt/ZrO 2 catalyst, which was attributed to the experimentally observed aggregation of Pt nanoparticles.

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          Most cited references54

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          Synthesis of transportation fuels from biomass: chemistry, catalysts, and engineering.

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            Thermally stable single-atom platinum-on-ceria catalysts via atom trapping

            Catalysts based on single atoms of scarce precious metals can lead to more efficient use through enhanced reactivity and selectivity. However, single atoms on catalyst supports can be mobile and aggregate into nanoparticles when heated at elevated temperatures. High temperatures are detrimental to catalyst performance unless these mobile atoms can be trapped. We used ceria powders having similar surface areas but different exposed surface facets. When mixed with a platinum/aluminum oxide catalyst and aged in air at 800°C, the platinum transferred to the ceria and was trapped. Polyhedral ceria and nanorods were more effective than ceria cubes at anchoring the platinum. Performing synthesis at high temperatures ensures that only the most stable binding sites are occupied, yielding a sinter-resistant, atomically dispersed catalyst.
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              Activation of surface lattice oxygen in single-atom Pt/CeO2for low-temperature CO oxidation

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                Author and article information

                Journal
                ACS Catal
                ACS Catal
                cs
                accacs
                ACS Catalysis
                American Chemical Society
                2155-5435
                16 September 2019
                01 November 2019
                : 9
                : 11
                : 9953-9963
                Affiliations
                []Chemical Engineering Group, Engineering and Technology Institute Groningen, University of Groningen , Nijenborgh 4, 9747 AG Groningen, The Netherlands
                []Electron Microscopy for Materials Science, University of Antwerp , Gronenenborgerlaan 171, 2020 Antwerp, Belgium
                [§ ]Advanced Production Engineering Group, Engineering and Technology Institute Groningen, University of Groningen , Nijenborgh 4, 9747 AG Groningen, The Netherlands
                Author notes
                Article
                10.1021/acscatal.9b02139
                7493308
                77e90667-72ad-4565-8a29-6e33ac96e15f
                Copyright © 2019 American Chemical Society

                This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.

                History
                : 23 May 2019
                : 30 August 2019
                Categories
                Research Article
                Custom metadata
                cs9b02139
                cs9b02139

                glycerol,lactic acid,pt catalyst,transfer hydrogenation,cyclohexene

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