4.7 Article

Carbon-catalyzed oxygen-mediated dehydrogenation of formaldehyde in alkaline solution for efficient hydrogen production

Journal

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 47, Issue 65, Pages 27877-27886

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2022.06.134

Keywords

Carbon catalysts; Dehydrogenation; Oxygen-mediated catalysis; Surface defects; Formaldehyde

Funding

  1. National Natural Science Foundation of China [21872123, 22172143]
  2. National Research Foundation of Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme

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We report an efficient process for dehydrogenating formaldehyde in alkaline solution using carbon nanotubes as catalysts with the involvement of molecular O-2 in a unique reaction mechanism. The superior catalytic performance of carbon nanotubes is attributed to their sp(2)-carbon-rich surface, hydrophilicity, and abundant surface defects, which serve as the most plausible active sites. The activation of adsorbed molecular oxygen on carbon nanotubes leading to peroxide species is found to be crucial for C-H activation and efficient hydrogen production. The cost-effective carbon-based dehydrogenation catalysts provide new opportunities for the development of novel liquid organic hydrogen carrier technologies.
We report an efficient process to dehydrogenate formaldehyde in alkaline solution, catalyzed by carbon nanotubes (CNTs) via a unique reaction mechanism involving molecular O-2. The superior catalytic performance of carbon nanotubes (CNTs) compared to the other carbon-based catalysts is attributed to their sp(2)-carbon-rich surface, hydrophilicity and abundant surface defects, which are the most plausible active sites. Peroxide species originating from the activation of adsorbed molecular oxygen on the CNTs is found to be a key to C-H activation, leading to efficient hydrogen production. The cost-effective carbon-based dehydrogenation catalysts offer new opportunities to the development of novel liquid organic hydrogen carrier technologies. (C) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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