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    Ni–Sn-Supported ZrO2 Catalysts Modified by Indium for Selective CO2 Hydrogenation to Methanol

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    Type
    Article
    Authors
    Hengne, Amol Mahalingappa
    Samal, Akshaya Kumar cc
    Enakonda, Linga
    Harb, Moussab cc
    Gevers, Lieven
    Anjum, Dalaver H. cc
    Hedhili, Mohamed N. cc
    Saih, Youssef
    Huang, Kuo-Wei cc
    Basset, Jean-Marie cc
    KAUST Department
    Chemical Science Program
    Electron Microscopy
    Homogeneous Catalysis Laboratory (HCL)
    Imaging and Characterization Core Lab
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Surface Science
    Date
    2018-04-02
    Online Publication Date
    2018-04-02
    Print Publication Date
    2018-04-30
    Permanent link to this record
    http://hdl.handle.net/10754/627526
    
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    Show full item record
    Abstract
    Ni and NiSn supported on zirconia (ZrO2) and on indium (In)-incorporated zirconia (InZrO2) catalysts were prepared by a wet chemical reduction route and tested for hydrogenation of CO2 to methanol in a fixed-bed isothermal flow reactor at 250 °C. The mono-metallic Ni (5%Ni/ZrO2) catalysts showed a very high selectivity for methane (99%) during CO2 hydrogenation. Introduction of Sn to this material with the following formulation 5Ni5Sn/ZrO2 (5% Ni-5% Sn/ZrO2) showed the rate of methanol formation to be 0.0417 μmol/(gcat·s) with 54% selectivity. Furthermore, the combination NiSn supported on InZrO2 (5Ni5Sn/10InZrO2) exhibited a rate of methanol formation 10 times higher than that on 5Ni/ZrO2 (0.1043 μmol/(gcat·s)) with 99% selectivity for methanol. All of these catalysts were characterized by X-ray diffraction, high-resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), X-ray photoelectron spectroscopy, CO2-temperature-programmed desorption, and density functional theory (DFT) studies. Addition of Sn to Ni catalysts resulted in the formation of a NiSn alloy. The NiSn alloy particle size was kept in the range of 10–15 nm, which was evidenced by HRTEM study. DFT analysis was carried out to identify the surface composition as well as the structural location of each element on the surface in three compositions investigated, namely, Ni28Sn27, Ni18Sn37, and Ni37Sn18 bimetallic nanoclusters, and results were in agreement with the STEM and electron energy-loss spectroscopy results. Also, the introduction of “Sn” and “In” helped improve the reducibility of Ni oxide and the basic strength of catalysts. Considerable details of the catalytic and structural properties of the Ni, NiSn, and NiSnIn catalyst systems were elucidated. These observations were decisive for achieving a highly efficient formation rate of methanol via CO2 by the H2 reduction process with high methanol selectivity.
    Citation
    Hengne AM, Samal AK, Enakonda LR, Harb M, Gevers LE, et al. (2018) Ni–Sn-Supported ZrO2 Catalysts Modified by Indium for Selective CO2 Hydrogenation to Methanol. ACS Omega 3: 3688–3701. Available: http://dx.doi.org/10.1021/acsomega.8b00211.
    Sponsors
    We are thankful for the financial support from the King Abdullah University of Science and Technology.
    Publisher
    American Chemical Society (ACS)
    Journal
    ACS Omega
    DOI
    10.1021/acsomega.8b00211
    Additional Links
    https://pubs.acs.org/doi/10.1021/acsomega.8b00211
    ae974a485f413a2113503eed53cd6c53
    10.1021/acsomega.8b00211
    Scopus Count
    Collections
    Articles; Imaging and Characterization Core Lab; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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