Abstract
Meeting ambitious net-zero targets will require the replacement of marine fossil fuels with sustainable alternatives such as dimethyl ether (DME). DME is non-toxic, can be fully produced via a circular carbon economy and can be rapidly deployed due to its compatibility with existing liquid petroleum gas infrastructure. One-pot production of DME from CO2via a methanol intermediate is achieved by combining redox and Brønsted or Lewis acid sites. Herein, we have synthesised, characterised and tested a variety of bifunctional CuZnO/silicoaluminophosphate catalysts for the one-pot production of DME. A range of synthetic approaches were employed to combine the redox and acidic functionalities in order to derive synthesis-structure-property correlations to guide the design of improved catalysts. We found that a CuZnO/SAPO-34 catalyst made via impregnation and drying can achieve 80% DME selectivity with no detectable toxic CO by-product formation. High acid site abundance resulted in extensive dehydration of the intermediate methanol, which increased localised water production, suppressing the CO-forming reverse water gas shift reaction and thus yielding exceptional DME selectivity that is amongst the highest in literature.
Original language | English |
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Pages (from-to) | 3853-3863 |
Number of pages | 11 |
Journal | Catalysis Science and Technology |
Volume | 14 |
Issue number | 14 |
Early online date | 2 Apr 2024 |
DOIs | |
Publication status | Published - 21 Jul 2024 |
Funding
MGW would like to thank the University of Southampton and the Southampton Marine and Maritime Institute for their funding. We would also like to thank: HarwellXPS for XPS data collection which was performed at EPSRC National Facility for XPS (\u2018HarwellXPS\u2019), operated by Cardiff University and UCL, under contract No. PR16195, UK Catalysis Hub block allocation group for XAFS beamtime (SP29271), Dr Matthew Cooper at the School of Ocean and Earth Science at the University of Southampton for their help with ICP-MS analysis, Patricia Goggin, Regan Doherty and the wider team at the Biological Imaging Unit at the University Hospital Southampton for their help with TEM imaging and Professor John Langley and Dr Julie Herniman for their help with GC\u2013MS analysis.
Funders | Funder number |
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University of Southampton | |
Southampton Marine and Maritime Institute |
ASJC Scopus subject areas
- Catalysis