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    Single cobalt sites in mesoporous N-doped carbon matrix for selective catalytic hydrogenation of nitroarenes

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    Type
    Article
    Authors
    Sun, Xiaohui
    Olivos-Suarez, Alma I.
    Osadchii, Dmitrii
    Romero, Maria Jose Valero
    Kapteijn, Freek cc
    Gascon, Jorge cc
    KAUST Department
    Chemical Engineering Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2017-11-20
    Online Publication Date
    2017-11-20
    Print Publication Date
    2018-01
    Permanent link to this record
    http://hdl.handle.net/10754/626185
    
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    Abstract
    A supported cobalt catalyst with atomically dispersed Co-Nx sites (3.5 wt% Co) in a mesoporous N-doped carbon matrix (named Co@mesoNC) is synthesized by hydrolysis of tetramethyl orthosilicate (TMOS) in a Zn/Co bimetallic zeolitic imidazolate framework (BIMZIF(Co,Zn)), followed by high-temperature pyrolysis and SiO2 leaching. A combination of TEM, XRD XPS and X-ray absorption spectroscopy studies confirm the absence of cobalt nanoparticles and indicate that these highly dispersed cobalt species are present in the form of Co-Nx. The exclusive formation of Co-Nx sites in the carbon matrix is attributed to the presence of a large amount of Zn and N in the BIMZIF precursor together with the presence of SiO2 in the pore space of this framework, extending the initial spatial distance between cobalt atoms and thereby impeding their agglomeration. The presence of SiO2 during high-temperature pyrolysis is proven crucial to create mesoporosity and a high BET area and pore volume in the N-doped carbon support (1780 m2 g−1, 1.54 cm3 g−1). This heterogeneous Co@mesoNC catalyst displays high activity and selectivity (>99%) for the selective hydrogenation of nitrobenzene to aniline at mild conditions (0.5–3 MPa, 343–383 K). When more challenging substrates (functionalized nitroarenes) are hydrogenated, the catalyst Co@mesoNC displays an excellent chemoselectivity to the corresponding substituted anilines.The presence of mesoporosity improves mass transport of reactants and/or products and the accessibility of the active Co-Nx sites, and greatly reduces deactivation due to fouling.
    Citation
    Sun X, Olivos-Suarez AI, Osadchii D, Romero MJV, Kapteijn F, et al. (2018) Single cobalt sites in mesoporous N-doped carbon matrix for selective catalytic hydrogenation of nitroarenes. Journal of Catalysis 357: 20–28. Available: http://dx.doi.org/10.1016/j.jcat.2017.10.030.
    Sponsors
    We thank for the support from the Dutch-Belgian program for access to the BM26A in ESRF, Grenoble. We thank A. Dikhtiarenko for help in the design of the graphical abstract. Xiaohui Sun acknowledges financial support from China Scholarship Council (CSC).
    Publisher
    Elsevier BV
    Journal
    Journal of Catalysis
    DOI
    10.1016/j.jcat.2017.10.030
    Additional Links
    http://www.sciencedirect.com/science/article/pii/S0021951717303901
    ae974a485f413a2113503eed53cd6c53
    10.1016/j.jcat.2017.10.030
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Engineering Program; KAUST Catalysis Center (KCC)

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