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Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C-H Activation

Title
Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C-H Activation
Authors
Xie, JiahanKammert, James D.Kaylor, NicholasZheng, Jonathan W.Choi, EunjinPham, Hien N.Sang, XiahanStavitski, EliAttenkofer, KlausUnocic, Raymond R.Datye, Abhaya K.Davis, Robert J.
Issue Date
2018-05
Citation
ACS Catalysis, 8(5), 3875-3884
Type
Article
Article Type
Article
Keywords
Activation analysisCarbonCatalyst activityChemical activationCopper compoundsDehydrogenationDoping (additives)Positive ionsPropaneThermodynamic stabilityX ray absorption spectroscopyAlcohol oxidationC-h activationCoordination environmentHeterogeneous catalystIn-situ XASN-dopedNon-precious metalsPropane dehydrogenationCobalt compounds
ISSN
2155-5435
Abstract
Atomically dispersed Co(II) cations coordinated to nitrogen in a carbon matrix (Co-N-C) catalyze oxidative dehydrogenation of benzyl alcohol in water with a specific activity approaching that of supported Pt nanoparticles. Whereas Cu(II) cations in N-doped carbon also catalyze the reaction, they are about an order of magnitude less active compared with Co(II) cations. Results from X-ray absorption spectroscopy suggest that oxygen is also bound to N-coordinated Co(II) sites but that it can be partially removed by H2 treatments at 523-750 K. The N-coordinated Co(II) sites remained cationic in H2 up to 750 K, and these stable sites were demonstrated to be active for propane dehydrogenation. In situ characterization of Cu(II) in N-doped carbon revealed that reduction of the metal in H2 started at about 473 K, indicating a much lower thermal stability of Cu(II) in H2 relative to Co(II). The demonstrated high catalytic activity and thermal stability of Co-N-C in reducing environments suggests that this material may have broad utility in a variety of catalytic transformations. © 2018 American Chemical Society.
URI
http://hdl.handle.net/20.500.11750/8982
DOI
10.1021/acscatal.8b00141
Publisher
American Chemical Society
Files:
There are no files associated with this item.
Collection:
ETC1. Journal Articles


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