From the journal Digital Discovery Peer review history

21-Apr-2024

Dear Dr Gregoire:

Manuscript ID: DD-ART-02-2024-000061
TITLE: Accelerated screening of gas diffusion electrodes for carbon dioxide reduction

Thank you for your submission to Digital Discovery, published by the Royal Society of Chemistry. I sent your manuscript to reviewers and I have now received their reports which are copied below. (Apologies for the long time in review; an earlier reviewer asked for extensions and finally failed to return a report, requiring us to find an alternate.)

After careful evaluation of your manuscript and the reviewers’ reports, I will be pleased to accept your manuscript for publication after minor revisions.

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I look forward to receiving your revised manuscript.

Yours sincerely,
Dr Joshua Schrier
Associate Editor, Digital Discovery

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Reviewer 1

Jones et al. present an interesting test stand to expedite the testing of gas diffusion electrode catalysts. I see this work to be of great importance for the acceleration of testing in the area of CO2 reduction and heterogenous catalysis in general. As the authors state there is a great reduction of time in the setup/exchange of the catalyst between tests and the rather complex procedure outlined in the supplementary information I believe it would be great for readers to maybe also have a brief video or photo series that outlines the expedited assembly process. In the battery field there has been a similar trend where initially the EL-Cell streamlined the assembly process of cells (and I believe they even offer residual gas analysis options) up until folks started to automate cell assembly completely. Not a necessity but an option could be to ask someone to assemble a GDE the "old way" and compare. Some additional
All in all I think this is a great paper, well written, and very concise so more or less publish as is (with the addition of some explanatory panels how the process looks or compares to conventional assembly).

Reviewer 2

The article introduces the Automated Gas Diffusion Electrode (AutoGDE) instrument developed by the Gregoire group. Overall, it is a commendable piece and serves as an excellent demonstration of DIY hardware. One aspect I would appreciate from the authors is commentary within the text regarding comparisons to existing setups. For instance, are there commercial alternatives available, and if so, how much cost savings does the DIY route offer? Alternatively, if there are no commercial alternatives, how much throughput enhancement does the automation provide?

Moreover, I was specifically tasked by the editor to provide feedback on the manuscript's characteristics concerning the hardware nature of the contributions, including the completeness of instructions and clarity. Upon reflection, I questioned whether I could replicate the setup based solely on the manuscript and supporting information. Unfortunately, the absence of assembly instructions and reliance on external repositories such as GitHub hindered this possibility. While incorporating all this information into the manuscript may not significantly benefit readers, given the requisite domain knowledge needed to conduct the experiments, it's worth noting that hardware descriptions can be broadly categorized into two types: those expected to be frequently replicated (e.g., automated syringes, dispensers, 3D printers) and those that are highly specialized and less likely to be replicated. I consider the AutoGDE to fall into the latter category, and therefore, providing specific "Ikea-style" assembly instructions could burden the authors unnecessarily.

That said, I believe some of the technical drawings from the repository should be included in the supporting information. This would offer readers an overview of the project's complexity and streamline the reading experience by consolidating relevant materials in one place, rather than requiring them to navigate between the paper, supplementary information, and GitHub repository.

This text has been copied from the PDF response to reviewers and does not include any figures, images or special characters

REVIEWER REPORT(S):
Referee: 1

Comments to the Author

Jones et al. present an interesting test stand to expedite the testing of gas diffusion electrode catalysts. I see this work to be of great importance for the acceleration of testing in the area of CO2 reduction and heterogenous catalysis in general. As the authors state there is a great reduction of time in the setup/exchange of the catalyst between tests and the rather complex procedure outlined in the supplementary information I believe it would be great for readers to maybe also have a brief video or photo series that outlines the expedited assembly process. In the battery field there has been a similar trend where initially the EL-Cell streamlined the assembly process of cells (and I believe they even offer residual gas analysis options) up until folks started to automate cell assembly completely. Not a necessity but an option could be to ask someone to assemble a GDE the "old way" and compare.
Response:
Thank you for the positive assessment and recommendations. We have added a comparison in the time required for manual vs AutoGDE cell assembly and electrolyte management, as detailed in response to Rev 2 below.

All in all I think this is a great paper, well written, and very concise so more or less publish as is (with the addition of some explanatory panels how the process looks or compares to conventional assembly).

Response: This is an excellent suggestion. We have added a new section “Comparison of operations between conventional and AutoGDE” to the SI that includes photographs of a traditional GDE and a commentary on the similarities and difference in cell assembly between the traditional cell and AutoGDE platform.

Referee: 2

Comments to the Author

The article introduces the Automated Gas Diffusion Electrode (AutoGDE) instrument developed by the Gregoire group. Overall, it is a commendable piece and serves as an excellent demonstration of DIY hardware. One aspect I would appreciate from the authors is commentary within the text regarding comparisons to existing setups. For instance, are there commercial alternatives available, and if so, how much cost savings does the DIY route offer? Alternatively, if there are no commercial alternatives, how much throughput enhancement does the automation provide?

Response: We are not aware of any commercial options. The main benefit of the automation is the acceleration of sample loading, and the ability to conduct an experimental protocol without human intervention. Thank you for noting that we should highlight these points in the paper, which we have done in conjunction with a numerical comparison of our Faradaic efficiencies with literature values in the following new text:

Although CO2RR performance on GDE could vary among electrochemical cell designs due to variation in, for example, mass transport and current distribution,19 our AutoGDE produces CO2RR product distributions commensurate with traditional Cu-based GDEs. To quantitatively compare Faradaic efficiencies (FE), we consider the results acquired near -1.1 V vs RHE, a potential commonly used to evaluate Cu catalyst in bicarbonate electrolytes due to the prevalence of C2+ products over H2. Our results of 48% FE toward C2+ products and 14% for H2 are commensurate with the literature values of 40% and 15%, respectively (see Table S2).20

Regarding the acceleration in experiment throughput, the time spent acquiring electrochemical data can be considered to be independent of the level of experiment automation. Automation shortens the time spent on other experiment steps, with ancillary benefits including increased reproducibility and robust data tracking. For the AutoGDE demonstration reported herein, there are 2 primary experiment preparation steps. The first step is the assembly of the electrochemical reactor with a new GDE sample, which for a traditional GDE experiment comparable to those presented herein takes 15-25 min due to the multi-step manual cell assembly. The equivalent time on the AutoGDE is less than 1 min, providing an approximate 20-fold acceleration. Second, electrolyte handling involves cell cleaning and (re)filling electrolyte, which occurs prior each electrochemical experiment for which independent liquid product characterization is desired, as well as archiving of the electrolytes for subsequent liquid product detection. These liquid handling tasks require at least 10 minutes of human researcher time with traditional methods, while AutoGDE reduces the time to 3 min and does not require human intervention to manage the electrolyte (or to subsequently start an electrochemical experiment). The overall increase of experiment throughput must be ascertained for a given electrochemical testing protocol and the availability of human researchers for conducting multiple experiments.

Moreover, I was specifically tasked by the editor to provide feedback on the manuscript's characteristics concerning the hardware nature of the contributions, including the completeness of instructions and clarity. Upon reflection, I questioned whether I could replicate the setup based solely on the manuscript and supporting information. Unfortunately, the absence of assembly instructions and reliance on external repositories such as GitHub hindered this possibility. While incorporating all this information into the manuscript may not significantly benefit readers, given the requisite domain knowledge needed to conduct the experiments, it's worth noting that hardware descriptions can be broadly categorized into two types: those expected to be frequently replicated (e.g., automated syringes, dispensers, 3D printers) and those that are highly specialized and less likely to be replicated. I consider the AutoGDE to fall into the latter category, and therefore, providing specific "Ikea-style" assembly instructions could burden the authors unnecessarily.

That said, I believe some of the technical drawings from the repository should be included in the supporting information. This would offer readers an overview of the project's complexity and streamline the reading experience by consolidating relevant materials in one place, rather than requiring them to navigate between the paper, supplementary information, and GitHub repository.

Response: Thank you for this recommendation. We created a new SI section “Abridged description of AutoGDE assembly” and pulled in the key visuals from the repository.

27-Apr-2024

Dear Dr Gregoire:

Manuscript ID: DD-ART-02-2024-000061.R1
TITLE: Accelerated screening of gas diffusion electrodes for carbon dioxide reduction

Thank you for submitting your revised manuscript to Digital Discovery. I am pleased to accept your manuscript for publication in its current form.

You will shortly receive a separate email from us requesting you to submit a licence to publish for your article, so that we can proceed with the preparation and publication of your manuscript.

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By publishing your article in Digital Discovery, you are supporting the Royal Society of Chemistry to help the chemical science community make the world a better place.

With best wishes,

Dr Joshua Schrier
Associate Editor, Digital Discovery


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