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Photoelectrochemical hybrid cell for unbiased CO2 reduction coupled to alcohol oxidation

Nature Synthesis volume 1, pages 77–86 (2022)Cite this article

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Abstract

The reduction of CO2 to renewable fuels must be coupled to a sustainable oxidation process to devise a viable device that produces solar fuels. In photoelectrochemical cells, water oxidation to O2 is the predominant oxidation reaction and typically requires a pair of light absorbers or an applied bias voltage when coupled to CO2 reduction. Here, we report a bias-free photoelectrochemical device for simultaneous CO2 reduction to formate and alcohol oxidation to aldehyde in aqueous conditions. The photoanode is constructed by co-immobilization of a diketopyrrolopyrrole-based chromophore and a nitroxyl-based alcohol oxidation catalyst on a mesoporous TiO2 scaffold, which provides a precious-metal-free dye-sensitized photoanode. The photoanode is wired to a biohybrid cathode that consists of the CO2 reduction enzyme formate dehydrogenase integrated into a mesoporous indium tin oxide electrode. The bias-free cell delivers sustained photocurrents of up to 30 µA cm−2 under visible-light irradiation, which results in simultaneous aldehyde and formate production. Our results show that in the absence of an external bias, single light absorber photoelectrochemical cells can be used for parallel fuel production and chemical synthesis from CO2 and alcohol substrates.

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Fig. 1: PEC cell with molecular components.
Fig. 2: Synthesis and characterization of the dyes.
Fig. 3: PEC characterization of the photoanode.
Fig. 4: Simultaneous CO2 reduction and 4-MBA oxidation in a two-electrode mTiO2|STEMPO/DPP-CA||mITO|FDH PEC cell.

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Data availability

The data supporting the findings of the study are available in the paper and its Supplementary Information. Other source data supporting the findings of this study are available from the Cambridge data repository (https://doi.org/10.17863/CAM.76484). Source data are provided with this paper.

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Acknowledgements

We acknowledge support from an EPSRC PhD DTA studentship (EP/M508007/1, D.A.-G.), the Christian Doppler Research Association (Austrian Federal Ministry for Digital and Economic Affairs and the National Foundation for Research, Technology and Development) and the OMV Group (M.A.B., J.W. and E.R.), an ERC Consolidator Grant ‘MatEnSAP’ (682833; D.A.-G., E.E.M. and E.R.), the Endeavour Scholarship Scheme (M.A.B.), the German National Academy of Sciences Leopoldina for a postdoctoral fellowship (LPDS 2018-04, A.E.), Fundação para a Ciência e Tecnologia (Portugal) for fellowship SFRH/BD/116515/2016 (A.R.O.), grant PTDC/BII-BBF/2050/2020 (I.A.C.P.) and R&D unit MOSTMICRO-ITQB (UIDB/04612/2020 and UIDP/04612/2020). J.W. gratefully acknowledges support from R. Fischer and the Deutsche Forschungsgemeinschaft (grant no. FI 502/43-1). We thank Q. Wang, N. Kornienko, C. Pichler and A. Wagner for helpful discussions. We also thank N. Heidary and K. Ly for their help in preparing the artwork. We appreciate suggestions and comments on the manuscript from T. Li and Q. Wang.

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Authors and Affiliations

  1. Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK

    Daniel Antón-García, Esther Edwardes Moore, Mark A. Bajada, Annika Eisenschmidt, Julien Warnan & Erwin Reisner

  2. Instituto de Tecnologia Química e Biológica António Xavier, Universidade Nova de Lisboa, Oeiras, Portugal

    Ana R. Oliveira & Inês A. C. Pereira

  3. Chemistry Department, Technische Universität München, Garching, Germany

    Julien Warnan

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Contributions

D.A.-G., J.W. and E.R. designed the project. D.A.-G. synthesized and characterized the DPP chromophores and the TEMPO-based catalyst. D.A.-G. and A.E. performed the DFT calculations and analysed the data. D.A.-G. and M.A.B. designed and characterized the alcohol oxidation photoanode, and carried out the PEC experiments of the photoanode. E.E.M. designed and characterized the CO2 reduction cathode. D.A.-G. and E.E.M. carried out the PEC experiments of the two-electrode cell, and analysed the data. A.R.O. and I.A.C.P. expressed, purified and characterized FDH. D.A.-G., J.W. and E.R. wrote the manuscript with contributions and discussions from all the authors. E.R. and J.W. supervised the research work.

Corresponding authors

Correspondence to Julien Warnan or Erwin Reisner.

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Peer review information Nature Synthesis thanks Wenzhen Li and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Alison Stoddart was the primary editor on this article and managed its editorial process and peer review in collaboration with the rest of the editorial team.

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Supplementary Methods, Tables 1–16, Figs. 1–30 and References 1–11.

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Antón-García, D., Edwardes Moore, E., Bajada, M.A. et al. Photoelectrochemical hybrid cell for unbiased CO2 reduction coupled to alcohol oxidation. Nat Synth 1, 77–86 (2022). https://doi.org/10.1038/s44160-021-00003-2

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