The rewiring of photosynthetic biomachineries to electrodes is a forward-looking semi-artificial route for sustainable bio-electricity and fuel generation. Currently, it is unclear how the electrode and biomaterial interface can be designed to meet the complex requirements for high biophotoelectrochemical performance. Here we developed an aerosol jet printing method for generating hierarchical electrode structures using indium tin oxide nanoparticles. We printed libraries of micropillar array electrodes varying in height and submicrometre surface features, and studied the energy/electron transfer processes across the bio-electrode interfaces. When wired to the cyanobacterium Synechocystis sp. PCC 6803, micropillar array electrodes with microbranches exhibited favourable biocatalyst loading, light utilization and electron flux output, ultimately almost doubling the photocurrent of state-of-the-art porous structures of the same height. When the micropillars’ heights were increased to 600 µm, milestone mediated photocurrent densities of 245 µA cm–2 (the closest thus far to theoretical predictions) and external quantum efficiencies of up to 29% could be reached. This study demonstrates how bio-energy from photosynthesis could be more efficiently harnessed in the future and provide new tools for three-dimensional electrode design.
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Nano-Micro Letters Open Access 13 July 2023
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All data used in this paper are available via the Apollo repository (https://doi.org/10.17863/CAM.80096) or on GitHub (https://github.com/JLawrence96/MicropillarArrayElectrodes).
All code used in this paper are available via the Apollo respository (https://doi.org/10.17863/CAM.80096) or on GitHub (https://github.com/JLawrence96/MicropillarArrayElectrodes).
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This work was supported by the Biotechnology and Biological Sciences Research Council (BB/M011194/1 to J.M.L., BB/R011923/1 to J.Z. and X.C.), the Cambridge Trust (L.T.W.) and the Isaac Newton Trust (SCHERTEL SNSF3 to L.S.). S.K.-N. is grateful for support from a European Research Council (ERC) Starting Grant (ERC-2014-STG-639526, NANOGEN). S.K.-N. and Q.J. acknowledge support from the EPSRC Centre of Advanced Materials for Integrated Energy Systems (CAM-IES) (grant EP/P007767/1). We thank H. Lloyd-Laney and E. Kitson for helpful discussions in statistical analysis. We thank N. Plumeré and H. Li for helpful discussions in electrochemistry. We thank P. J. Bártolo and F. Liu for helpful discussions in 3D bioprinting.
The authors declare no competing interests.
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Chen, X., Lawrence, J.M., Wey, L.T. et al. 3D-printed hierarchical pillar array electrodes for high-performance semi-artificial photosynthesis. Nat. Mater. 21, 811–818 (2022). https://doi.org/10.1038/s41563-022-01205-5
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