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Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C-H Activation
- Atomically Dispersed Co and Cu on N-Doped Carbon for Reactions Involving C-H Activation
- Xie, Jiahan; Kammert, James D.; Kaylor, Nicholas; Zheng, Jonathan W.; Choi, Eunjin; Pham, Hien N.; Sang, Xiahan; Stavitski, Eli; Attenkofer, Klaus; Unocic, Raymond R.; Datye, Abhaya K.; Davis, Robert J.
- Issue Date
- ACS Catalysis, 8(5), 3875-3884
- Article Type
- Activation analysis; Carbon; Catalyst activity; Chemical activation; Copper compounds; Dehydrogenation; Doping (additives); Positive ions; Propane; Thermodynamic stability; X ray absorption spectroscopy; Alcohol oxidation; C-h activation; Coordination environment; Heterogeneous catalyst; In-situ XAS; N-doped; Non-precious metals; Propane dehydrogenation; Cobalt compounds
- 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.
- American Chemical Society
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