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    Structure-activity relationships in metal organic framework derived mesoporous nitrogen-doped carbon containing atomically dispersed iron sites for CO2 electrochemical reduction

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    Sun et al.pdf
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    Type
    Article
    Authors
    Sun, Xiaohui
    Wang, Riming cc
    Ould-Chikh, Samy cc
    Osadchii, Dmitrii
    Li, Guanna
    Aguilar, Antonio
    Hazemann, Jean-louis
    Kapteijn, Freek cc
    Gascon, Jorge cc
    KAUST Department
    Chemical Engineering Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2019-09-25
    Online Publication Date
    2019-09-25
    Print Publication Date
    2019-10
    Permanent link to this record
    http://hdl.handle.net/10754/656926
    
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    Abstract
    Mesoporous nitrogen-doped carbon nanoparticles with atomically dispersed iron sites (named mesoNC-Fe) are synthesized via high-temperature pyrolysis of an Fe containing ZIF-8 MOF. Hydrolysis of tetramethyl orthosilicate (TMOS) in the MOF framework prior to pyrolysis plays an essential role in maintaining a high surface area during the formation of the carbon structure, impeding the formation of iron (oxide) nanoparticles. To gain inside on the nature of the resulting atomically dispersed Fe moieties, HERFD-XANES, EXAFS and valence-to-core X-ray emission spectroscopies have been used. The experimental spectra (both XAS and XES) combined with theoretical calculations suggest that iron has a coordination sphere including a porphyrinic environment and OH/H2O moieties responsible for the high activity in CO2 electroreduction. DFT calculations demonstrate that CO formation is favored in these structures because the free energy barriers of *COOH formation are decreased and the adsorption of *H is impeded. The combination of such a unique coordination environment with a high surface area in the carbon structure of mesoNC-Fe makes more active sites accessible during catalysis and promotes CO2 electroreduction.
    Citation
    Sun, X., Wang, R., Ould-Chikh, S., Osadchii, D., Li, G., Aguilar, A., … Gascon, J. (2019). Structure-activity relationships in metal organic framework derived mesoporous nitrogen-doped carbon containing atomically dispersed iron sites for CO2 electrochemical reduction. Journal of Catalysis, 378, 320–330. doi:10.1016/j.jcat.2019.09.013
    Sponsors
    We thank Alma I. Olivos Suarez for help in the design of the graphical abstract. Mauro Rovezzi is kindly thanked for the extraction of the X-ray emission spectra. Guanna Li thanks the NWO veni grant (no. 016.Veni.172.034). NWO surfsara is acknowledged for providing access to the supercomputer facilities.
    Publisher
    Elsevier BV
    Journal
    Journal of Catalysis
    DOI
    10.1016/j.jcat.2019.09.013
    Additional Links
    https://linkinghub.elsevier.com/retrieve/pii/S0021951719304439
    ae974a485f413a2113503eed53cd6c53
    10.1016/j.jcat.2019.09.013
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Engineering Program; KAUST Catalysis Center (KCC)

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