Photocatalytic Semi-Hydrogenation of Acetylene to Polymer-Grade Ethylene with Molecular and Metal-Organic Framework Cobaloximes

© 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - (2024) vom: 22. Okt., Seite e2408658
1. Verfasser: Stone, Aaron E B S (VerfasserIn)
Weitere Verfasser: Fortunato, Anna, Wang, Xijun, Saggioro, Edoardo, Snurr, Randall Q, Hupp, Joseph T, Arcudi, Francesca, Ðorđević, Luka
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article acetylene reduction hydrogenation metal–organic frameworks molecular catalysts photocatalysis
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520 |a The semi-hydrogenation of acetylene in ethylene-rich gas streams is a high-priority industrial chemical reaction for producing polymer-grade ethylene. Traditional thermocatalytic routes for acetylene reduction to ethylene, despite progress, still require high temperatures and high H2 consumption, possess relatively low selectivity, and use a noble metal catalyst. Light-powered strategies are starting to emerge, given that they have the potential to use directly the abundant and sustainable solar irradiation, but are ineffective. Here an efficient, >99.9% selective, visible-light powered, catalytic conversion of acetylene to ethylene is reported. The catalyst is a homogeneous molecular cobaloxime that operates in tandem with a photosensitizer at room temperature and bypasses the use of non-environmentally friendly and flammable H2 gas feed. The reaction proceeds through a cobalt-hydride intermediate with ≈100% conversion of acetylene under competitive (ethylene co-feed) conditions after only 50 min, and with no evolution of H2 or over-hydrogenation to ethane. The cobaloxime is further incorporated as a linker in a metal-organic framework; the result is a heterogeneous catalyst for the conversion of acetylene under competitive (ethylene co-feed) conditions that can be recycled up to six times and remains catalytically active for 48 h, before significant loss of performance is observed 
650 4 |a Journal Article 
650 4 |a acetylene reduction 
650 4 |a hydrogenation 
650 4 |a metal–organic frameworks 
650 4 |a molecular catalysts 
650 4 |a photocatalysis 
700 1 |a Fortunato, Anna  |e verfasserin  |4 aut 
700 1 |a Wang, Xijun  |e verfasserin  |4 aut 
700 1 |a Saggioro, Edoardo  |e verfasserin  |4 aut 
700 1 |a Snurr, Randall Q  |e verfasserin  |4 aut 
700 1 |a Hupp, Joseph T  |e verfasserin  |4 aut 
700 1 |a Arcudi, Francesca  |e verfasserin  |4 aut 
700 1 |a Ðorđević, Luka  |e verfasserin  |4 aut 
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773 1 8 |g year:2024  |g day:22  |g month:10  |g pages:e2408658 
856 4 0 |u http://dx.doi.org/10.1002/adma.202408658  |3 Volltext 
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