Browsing by Subject "Dehydrogenation"

Sort by: Order: Results:

Now showing items 1-2 of 2
  • Boom, Devin H. A.; de Boed, Ewoud J. J.; Nicolas, Emmanuel; Nieger, Martin; Ehlers, Andreas W.; Jupp, Andrew R.; Slootweg, J. Chris (2020)
    The reaction of the intramolecular frustrated Lewis pair (FLP) tBu2PCH2BPh2 with the amine-boranes NH3·BH3 and Me2NH·BH3 leads to the formation of the corresponding FLP-H2 adducts as well as novel five-membered heterocycles that result from capturing the in situ formed amino-borane by a second equivalent of FLP. The sterically more demanding tBu2PCH2BMes2 does not form such a five-membered heterocycle when reacted with Me2NH·BH3 and its H2 adduct liberates dihydrogen at elevated temperatures, promoting the metal-free catalytic dehydrogenation of amine-boranes.
  • Liu, Yanduo; Chen, Yihong; Jiang, Wenbin; Kong, Tingting; Camargo, Pedro H. C.; Gao, Chao; Xiong, Yujie (2022)
    Photocatalytic nonoxidative coupling of CH4 to multicarbon (C2+) hydrocarbons (e.g., C2H4) and H2 under ambient conditions provides a promising energy-conserving approach for utilization of carbon resource. However, as the methyl intermediates prefer to undergo self-coupling to produce ethane, it is a challenging task to control the selective conversion of CH4 to higher value-added C2H4. Herein, we adopt a synergistic catalysis strategy by integrating Pd-Zn active sites on visible light-responsive defective WO3 nanosheets for synergizing the adsorption, activation, and dehydrogenation processes in CH4 to C2H4 conversion. Benefiting from the synergy, our model catalyst achieves a remarkable C2+ compounds yield of 31.85 mu mol center dot g-1 center dot h-1 with an exceptionally high C2H4 selectivity of 75.3% and a stoichiometric H2 evolution. In situ spectroscopic studies reveal that the Zn sites promote the adsorption and activation of CH4 molecules to generate methyl and methoxy intermediates with the assistance of lattice oxygen, while the Pd sites facilitate the dehydrogenation of methoxy to methylene radicals for producing C2H4 and suppress overoxidation. This work demonstrates a strategy for designing efficient photocatalysts toward selective coupling of CH4 to higher value-added chemicals and highlights the importance of synergistic active sites to the synergy of key steps in catalytic reactions.