Journal
ACS CATALYSIS
Volume 8, Issue 5, Pages 3875-3884Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b00141
Keywords
heterogeneous catalyst; C-H activation; alcohol oxidation; propane dehydrogenation; nonprecious metal; N-doped carbon; in situ XAS; coordination environment
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Funding
- U.S. NSF [EEC-0813570, CBET-1157829]
- DOE Office of Science [DE-SC0012704]
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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 H-2 treatments at 523-750 K The N-coordinated Co(II) sites remained cationic in H-2 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 H-2 started at about 473 K, indicating a much lower thermal stability of Cu(II) in H-2 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.
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