Photoreforming of solid waste on 1 m2 scale under real- world conditions using single-source precursor-derived co-catalyst films Ariffin Bin Mohamad Annuar,1,† Subhajit Bhattacharjee,1,† Yongpeng Liu,1 Jonathan Slaughter,1,2 Clare P. Grey,1,2 Dominic S. Wright1,2 and Erwin Reisner1,* 1 Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, UK
2 Faraday Institution, Quad 1, Harwell Science and Innovation Campus, Didcot OX11 0RA, UK
† These authors have contributed equally to this work
*E-mail: reisner@ch.cam.ac.uk
Photocatalytic reforming can valorise biomass and plastic waste streams to generate clean H2 under ambient temperature and pressure. However, the fabrication of scalable photocatalyst (PC) sheets for this application is challenged by the need for high-temperature annealing, the use of binders and complex co-catalyst deposition routes. Here, we employ a [Co4Zr2O(OnPr)10(acac)4] single-source precursor (SSP) deposited on Al-doped SrTiO3 semiconductors and immobilised on glass supports for the facile fabrication of PC sheets using multiple deposition techniques, including high-throughput ambient-condition spray-coating. The PC sheets were applied for photoreforming feedstocks derived from cellulose and a real PET bottle, producing 0.21±0.03 and 0.07±0.01 μmol cm−2 h−1 of H2 from the respective feedstocks along with the value-added organics formate, acetate, glycolate and glycoaldehyde dimer. The versatility and scalability of the PC sheets is also shown from a cm2 to m2 scale, culminating in the first reported m2 demonstration of photoreforming of solid waste under real-world conditions. After 6 h of operation under natural sunlight with glucose or pre-treated cellulose substrates, the 1 m2 system achieved a maximum H2 production of 5.24 or 1.51 mmol m−2 with 2.68 or 1.50 mmol m−2 of formate and 1.76 or 0.94 mmol m−2 of acetate, respectively. A technoeconomic analysis was then performed based on the real-world demonstrations, showing for the first time a feasibility study on a concrete dataset obtained from a large-scale PC system, which resulted in a high but realistic estimated H2 cost of £0.93 mmol−1. This work provides new insights into the large-scale application of photocatalytic reforming and will guide future research towards achieving real-world implementation of these systems. References 1. Wang, Q. & Domen, K. Particulate Photocatalysts for Light-Driven Water Splitting: Mechanisms, Challenges, and Design Strategies. Chem. Rev. 120, 919–985 (2020). 2. Uekert, T., Bajada, M. A., Schubert, T., Pichler, C. M. & Reisner, E. Scalable Photocatalyst Panels for Photoreforming of Plastic, Biomass and Mixed Waste in Flow. ChemSusChem 14, 4190–4197 (2021). 3. Nishiyama, H. et al. Photocatalytic solar hydrogen production from water on a 100-m 2 scale. Nature 598, 304– 307 (2021). 4. Slaughter, J. et al. Synthesis of Heterometallic Zirconium Alkoxide Single-Source Precursors for Bimetallic Oxide Deposition. Inorg. Chem. 61, 19203–19219 (2022). 5. Uekert, T., Pichler, C. M., Schubert, T. & Reisner, E. Solar-driven reforming of solid waste for a sustainable future. Nat. Sustain. 4, 383–391 (2021).
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