Photocatalytic Removal of the Greenhouse Gas Nitrous Oxide by Liposomal Microreactors. (5th September 2022)

• Record Type: Journal Article
• Authors: Piper, Samuel E. H.; Casadevall, Carla; Reisner, Erwin; Clarke, Thomas A.; Jeuken, Lars J. C.; Gates, Andrew J.; Butt, Julea N.
• Is Part Of: Angewandte Chemie. Volume 134:Number 41(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-09-05
• Subjects: Carbon Dot -- Enzyme Catalysis -- Liposomes -- Nitrous Oxide -- Photochemistry; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202210572
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Nitrous oxide (N2 O) is a potent greenhouse and ozone‐reactive gas for which emissions are growing rapidly due to increasingly intensive agriculture. Synthetic catalysts for N2 O decomposition typically contain precious metals and/or operate at elevated temperatures driving a desire for more sustainable alternatives. Here we demonstrate self‐assembly of liposomal microreactors enabling catalytic reduction of N2 O to the climate neutral product N2 . Photoexcitation of graphitic N‐doped carbon dots delivers electrons to encapsulated N2 O Reductase enzymes via a lipid‐soluble biomolecular wire provided by the MtrCAB protein complex. Within the microreactor, electron transfer from MtrCAB to N2 O Reductase is facilitated by the general redox mediator methyl viologen. The liposomal microreactors use only earth‐abundant elements to catalyze N2 O removal in ambient, aqueous conditions. Abstract : Self‐assembled liposome microreactors mimic the spatial separation of redox reactions seen in respiration and photosynthesis. Catalytic reduction of the climate heating gas N2 O to benign N2 by encapsulated enzyme is driven by irradiation of external carbon dots through an electron transfer pathway defined by a membrane‐spanning cytochrome and redox‐cycling of internal methyl viologen.