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Parallel experiments in electrochemical CO2 reduction enabled by standardized analytics

Nature Catalysis volume 7, pages 742–752 (2024)Cite this article

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Abstract

Electrochemical CO2 reduction (eCO2R) is a promising strategy to transform detrimental CO2 emissions into sustainable fuels and chemicals. Key requirements for advancing this field are the development of analytical systems and of methods that are able to accurately and reproducibly assess the performance of catalysts, electrodes and electrolysers. Here we present a comprehensive analytical system for eCO2R based on commercial hardware, which captures data for >20 gas and liquid products with <5 min time resolution by chromatography, tracks gas flow rates, monitors electrolyser temperatures and flow pressures, and records electrolyser resistances and electrode surface areas. To complement the hardware, we develop an open-source software that automatically parses, aligns in time and post-processes the heterogeneous data, yielding quantities such as Faradaic efficiencies and corrected voltages. We showcase the system’s capabilities by performing measurements and data analysis on eight parallel electrolyser cells simultaneously.

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Fig. 1: Schematics of the comprehensive analytical system connected to a three-compartment electrochemical cell.
Fig. 2: GC and HPLC chromatograms of common eCO2R products.
Fig. 3: Data analysis plots automatically generated by our open-source software.
Fig. 4: Losses of volatile analytes from the catholyte analysed by GC and HPLC.
Fig. 5: Comprehensive dataset collected on a Cu GDE at 200 mA cm−2.
Fig. 6: Comprehensive analysis carried out on eight parallel electrolyser cells simultaneously.

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Data availability

Data used in this manuscript are freely available via Zenodo at https://doi.org/10.5281/zenodo.8319625 (ref. 54). Data for composing Fig. 3 are also part of an interactive example of automated data parsing and processing that can be accessed via Zenodo at https://doi.org/10.5281/zenodo.7941528 (ref. 32).

Code availability

The code used in this work is fully open source and available at https://dgbowl.github.io/ (ref. 33).

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Acknowledgements

This work has received funding from the ETH Board in the framework of the Joint Strategic Initiative ‘Synthetic Fuels from Renewable Resources’. This work was also supported by the NCCR Catalysis, a National Centre of Competence in Research funded by the Swiss National Science Foundation (grant no. 180544). We further acknowledge support by the Open Research Data Program of the ETH Board (project ‘PREMISE’: Open and Reproducible Materials Science Research). A.S. acknowledges funding from the Swiss National Science Foundation through the Ambizione grant PZ00P2_215992. We thank C. Spitz, S. Holmann and M. Maier from Agilent Technologies (Switzerland) for support with validating the chromatographic method. We thank N. Vetsch for help in coding the electrochemical data parser, and J. Viloria for support during electrochemical experiments. E. Querel is acknowledged for help with the ICP measurements. We also acknowledge the support of the Scientific Center for Optical and Electron Microscopy (ScopeM) of the ETH Zurich and of P. Zeng of ScopeM for the focused ion beam-SEM results. We also thank M. Mirolo of beamline ID31 at the European Synchrotron Radiation Facility (ESRF) for support with the synchrotron X-ray measurements.

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Authors and Affiliations

  1. Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland

    Alessandro Senocrate, Francesco Bernasconi, Peter Kraus, Nukorn Plainpan, Ulrich Sauter & Corsin Battaglia

  2. ETH Zürich, Department of Information Technology and Electrical Engineering, Zürich, Switzerland

    Alessandro Senocrate & Corsin Battaglia

  3. ETH Zürich, Department of Materials, Zürich, Switzerland

    Francesco Bernasconi & Corsin Battaglia

  4. Agilent Technologies (Switzerland), Basel, Switzerland

    Jens Trafkowski, Fabian Tolle & Thomas Weber

  5. EPFL, School of Engineering, Institute of Materials, Lausanne, Switzerland

    Corsin Battaglia

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  1. Alessandro Senocrate
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Contributions

A.S. designed, validated and assembled the hardware, performed the main electrochemical experiments and wrote the manuscript with input from all co-authors. F.B. contributed to the electrochemical experiments, validation of the method, assembly of the hardware and acquisition of the SEM images. P.K. wrote the open-source software and contributed to the data analysis. N.P. supported the data analysis effort and wrote the script required to analyse data from parallel cells. J.T., F.T. and T.W. supported the implementation of the online liquid sampling and liquid analysis. U.S. helped writing and debugging the open-source software. C.B. supervised the development of the project.

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Correspondence to Alessandro Senocrate.

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Nature Catalysis thanks Joel Ager III, Zhihao Cui and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Notes 1–10, Figs. 1–21 and Tables 1–11.

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Senocrate, A., Bernasconi, F., Kraus, P. et al. Parallel experiments in electrochemical CO2 reduction enabled by standardized analytics. Nat Catal 7, 742–752 (2024). https://doi.org/10.1038/s41929-024-01172-x

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