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Photoreforming of solid waste on 1 m2 scale using single-source precursor-derived co-catalyst films.

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Peer-reviewed

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Abstract

Photocatalytic reforming offers a route to valorize biomass and plastic waste into clean H2 under ambient conditions. However, the scalability of photocatalyst sheets is limited by high-temperature processing, binders and complex co-catalyst deposition. Here a [Co4Zr2O(O n Pr)10(acac)4] single-source precursor is deposited onto Al-doped SrTiO3 and immobilized on glass substrates to fabricate photocatalyst sheets using multiple techniques, including high-throughput spray coating. The resulting sheets enable photoreforming of cellulose- and polyethylene terephthalate-derived feedstocks, producing H2 alongside value-added organics such as formate, acetate, glycolate and glycolaldehyde dimer. The system is demonstrated from the centimeter- to meter-squared scale, culminating in a 1-m2 outdoor reactor operating under natural sunlight. After 6 h, H2 yields reached 5.24 and 1.51 mmol m-2 for glucose and pretreated cellulose, respectively, with concurrent formation of oxygenates. Techno-economic analysis based on real-world data estimates an H2 cost of £0.93 mmol-1. This work advances scalable photocatalytic reforming and provides a step towards practical deployment.

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Acknowledgements: This work was supported by the UK Department of Science, Innovation and Technology and the Royal Academy of Engineering Chair in Emerging Technologies program (CIET-2324-83 to E.R.), UK Research & Innovation (UKRI; ERC Advanced Grant EP/X030563/1 to ER), the Petronas Education Sponsorship Programme for Postgraduate Studies (to A.B.M.A.), the NanoDTC NanoFutures Leadership Award (to S.B.), the Leverhulme Early Career Fellowship (ECF-2024-230 to Y.L.), the Isaac Newton Trust (23.23(g) and 24.08(s) to Y.L.), the Swiss National Science Foundation Postdoc.Mobility Fellowship (P500PN_202908 to Y.L.) and the Faraday Institution (FIRG024 and FIRG064 to J.S., C.P.G. and D.S.W.); the Cambridge Royce Facilities (EP/P024947/1) and the Sir Henry Royce Institute (Equipment Access Scheme, EP/R00661X/1) for XPS data collection by S. Guan; and The Diamond Light Source Ltd, UK, for beamtime on B18 beamline (proposal no. SP42410). We acknowledge H. Greer for acquiring the TEM data (EPSRC grant (EP/P030467/1) for funding the TEM), S. Impey and M. Woolley for the construction of the large-scale photoreactor, A. Bond for acquiring and refining the single crystal X-ray diffraction data and C. Woo Lee and L. Chen for useful feedback on the manuscript.


Funder: Petronas Education Sponsorship Programme


Funder: Faraday Institution (FIRG024 and FIRG064)


Funder: Diamond Light Source Ltd, UK for beamtime on B18 beamline (proposal no: SP42410)

Journal Title

Nat Chem Eng

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Journal ISSN

2948-1198
2948-1198

Volume Title

3

Publisher

Springer Nature

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Except where otherwised noted, this item's license is described as http://creativecommons.org/licenses/by/4.0/
Sponsorship
Engineering and Physical Sciences Research Council (EP/P030467/1)
Engineering and Physical Sciences Research Council (EP/P024947/1)
Engineering and Physical Sciences Research Council (EP/R00661X/1)

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