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  Recycling of CO2 by Hydrogenation of Carbonate Derivatives to Methanol: Tuning Copper–Oxide Promotion Effects in Supported Catalysts

Kim, J., Pfänder, N., & Prieto, G. (2020). Recycling of CO2 by Hydrogenation of Carbonate Derivatives to Methanol: Tuning Copper–Oxide Promotion Effects in Supported Catalysts. ChemSusChem, 13(8), 2043-2052. doi:10.1002/cssc.202000166.

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 Creators:
Kim, Jonglack1, Author              
Pfänder, Norbert2, Author              
Prieto, Gonzalo1, Author              
Affiliations:
1Research Group Prieto, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2243639              
2Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              

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Free keywords: carbon dioxide fixation; copper; hydrogenation; nanoparticles; supported catalysts
 Abstract: The selective hydrogenation of organic carbonates to methanol is a relevant transformation to realize flexible processes for the recycling of waste CO2 with renewable H2 mediated by condensed carbon dioxide surrogates. Oxide‐supported copper nanoparticles are promising solid catalysts for this selective hydrogenation. However, essential for their optimization is to rationalize the prominent impact of the oxide support on performance. Herein, the role of Lewis acid centers, exposed on the oxide support at the periphery of the Cu nanoparticles, was systematically assessed. For the hydrogenation of propylene carbonate, as a model cyclic carbonate, the conversion rate, the apparent activation energy, and the selectivity to methanol correlate with the Lewis acidity of the coordinatively unsaturated cationic sites exposed on the oxide support. Lewis sites of markedly low and high electron‐withdrawing character promote unselective decarbonylation and decarboxylation reaction pathways, respectively. Supports exposing Lewis sites of intermediate acidity maximize the selectivity to methanol while inhibiting acid‐catalyzed secondary reactions of the propanediol product, and thus enable its recovery in cyclic processes of CO2 hydrogenation mediated by condensed carbonate derivatives. These findings help rationalize metal–support promotion effects that determine the performance of supported metal nanoparticles in this and other selective hydrogenation reactions of significance in the context of sustainable chemistry.

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Language(s): eng - English
 Dates: 2020-01-192020-02-152020-04-21
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/cssc.202000166
 Degree: -

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Title: ChemSusChem
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 13 (8) Sequence Number: - Start / End Page: 2043 - 2052 Identifier: ISSN: 1864-5631
CoNE: https://pure.mpg.de/cone/journals/resource/1864-5631