Show simple item record

dc.contributor.authorSun, Xiaohui
dc.contributor.authorOlivos-Suarez, Alma I.
dc.contributor.authorOsadchii, Dmitrii
dc.contributor.authorRomero, Maria Jose Valero
dc.contributor.authorKapteijn, Freek
dc.contributor.authorGascon, Jorge
dc.date.accessioned2017-11-21T11:18:54Z
dc.date.available2017-11-21T11:18:54Z
dc.date.issued2017-11-20
dc.identifier.citationSun 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.
dc.identifier.issn0021-9517
dc.identifier.doi10.1016/j.jcat.2017.10.030
dc.identifier.urihttp://hdl.handle.net/10754/626185
dc.description.abstractA 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.
dc.description.sponsorshipWe 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).
dc.publisherElsevier BV
dc.relation.urlhttp://www.sciencedirect.com/science/article/pii/S0021951717303901
dc.rightsNOTICE: this is the author’s version of a work that was accepted for publication in Journal of Catalysis. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Catalysis, [, , (2017-11-20)] DOI: 10.1016/j.jcat.2017.10.030 . © 2017. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.subjectNitroarene
dc.subjectHydrogenation
dc.subjectCo single atom
dc.subjectChemoselectivity
dc.titleSingle cobalt sites in mesoporous N-doped carbon matrix for selective catalytic hydrogenation of nitroarenes
dc.typeArticle
dc.contributor.departmentChemical Engineering Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalJournal of Catalysis
dc.eprint.versionPost-print
dc.contributor.institutionCatalysis Engineering, Department of Chemical Engineering, Delft University of Technology, Van der Maasweg 9, 2629 HZ Delft, The Netherlands
kaust.personOlivos-Suarez, Alma I.
kaust.personGascon, Jorge
refterms.dateFOA2019-11-20T00:00:00Z
dc.date.published-online2017-11-20
dc.date.published-print2018-01


Files in this item

Thumbnail
Name:
Sun et al..pdf
Size:
1.246Mb
Format:
PDF
Description:
Accepted Manuscript

This item appears in the following Collection(s)

Show simple item record