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Au Cluster-derived Electrocatalysts for CO2 Reduction

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Abstract

Metal clusters often exhibit superior chemical, electronic, and geometrical properties and can show exciting catalytic performance. The catalytic behaviour of the clusters is strongly affected by their size and composition, offering unique opportunities to fine-tune such materials for a specific application. In this study, atomically precise [Au6(dppp)4](NO3)2, [Au9(PPh3)8](NO3)3, [Au13(dppe)5Cl2]Cl3 and Au101(PPPh3)21Cl5 clusters were synthesised, characterised and their activity for electrocatalytic CO2 reduction is compared. These Au clusters were deposited onto carbon paper to serve as the cathode for the electrochemical reduction of CO2. The experimental studies suggest that the clusters remain intact upon deposition on the carbon paper but undergo agglomeration during CO2 electrolysis. The cluster-based catalysts demonstrated high selectivity (75%—90%) for CO production over hydrogen evolution reaction. Upon calcination, the activity of the cluster-based electrodes decreases, which can be attributed to the agglomeration of small clusters into larger bulk-like nanoparticles, as suggested by XPS, XAS and SEM.

Graphical Abstract

A series of phosphine-protected gold clusters supported on carbon paper were studied as CO2RR electrocatalysts. The CO2RR activity was dependent on their size and ligand density. Thermal annealing of the catalysts invariably lowered CO selectivity due to agglomeration of the clusters into larger nanoparticles.

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Availability of Data and Materials

The majority of data created during this study are available within this manuscript and its Supplementary Material. All other data is available upon reasonable request to the corresponding author.

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Acknowledgements

This research was undertaken on the X-ray absorption spectroscopy beamline at the Australian Synchrotron, part of ANSTO, grant M16325. The authors thank Dr Rosalie Hocking, Ms Brittany Kerr, and Mr Jaydon Meilak for their help in carrying out the experiments. SKS thanks the University of Canterbury for the UC Connect PhD scholarship.

Funding

SKS acknowledges the funding support of the UC Connect PhD scholarship.

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Authors and Affiliations

  1. School of Physical and Chemical Sciences, MacDiarmid Institute for Advanced Materials and Nanotechnology, University of Canterbury, Christchurch, New Zealand

    Shailendra Kumar Sharma & Vladimir B. Golovko

  2. Department of Chemical and Process Engineering, MacDiarmid Institute for Advanced Materials and Nanotechnology, University of Canterbury, Christchurch, New Zealand

    Shailendra Kumar Sharma, Hani Taleshi Ahangari & Aaron T. Marshall

  3. Australian Synchrotron, 800 Blackburn Rd, Clayton, VIC, 3168, Australia

    Bernt Johannessen

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Contributions

SKS: Methodology, Nanomaterial synthesis, Investigation, Formal analysis, Writing—original draft preparation, and leading the manuscript writing. HTA: Electrocatalysis measurements and subsequent analysis, Writing the relevant text in the original draft. BJ: Investigation. VBG: Methodology, Supervision, Manuscript review and editing. ATM: Methodology, Supervision, Manuscript review and editing.

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Correspondence to Shailendra Kumar Sharma, Vladimir B. Golovko or Aaron T. Marshall.

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Sharma, S.K., Ahangari, H.T., Johannessen, B. et al. Au Cluster-derived Electrocatalysts for CO2 Reduction. Electrocatalysis 14, 611–623 (2023). https://doi.org/10.1007/s12678-023-00821-2

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