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Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons

Published online by Cambridge University Press:  13 October 2025

Gad Licht
Affiliation:
Direct Air Capture LLC, North Venice, FL, USA
Kyle Hofstetter
Affiliation:
Carbon Corp, Calgary, AB, Canada
Stuart Licht*
Affiliation:
Direct Air Capture LLC, North Venice, FL, USA Carbon Corp, Calgary, AB, Canada Department of Chemistry, George Washington University, Washington, DC, USA
*
Corresponding author: Stuart Licht; Email: slicht@gwu.edu
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Abstract

This study explores the development and scale-up of an emerging carbon capture technology using molten carbonate electrolysis, which converts CO2 into high-value graphene nanocarbons (GNCs) and oxygen in a single step, offering a scalable and economically incentivized pathway to address global greenhouse gas emissions. Paths to large-scale carbon capture using molten carbonate electrolysis that splits CO2 into GNCs and O2 are studied and advanced. GNCs include carbon nanotubes, carbon nano-onions and other zero-, one-, two- and three-dimensional graphene nanoallotropes. The CO2 to carbon nanotechnology (C2CNT) carbon capture utilization process directly removes the greenhouse gas CO2 over a wide range of concentrations (from 400 ppm to pure CO2), incentivizing the capture by providing a value-added product. Scale-up of the original lab-scale discovery of the transition metal nucleated electrolytic splitting of CO2 to an industrial process is documented. The scale-up includes a three-order-of-magnitude increase in the size of the electrolysis electrodes, an increase in the individual electrolysis modules to 100-tonne CO2 annually, and a new industrial-scale production extraction unit separating the molten electrolyte from the GNC product. The molten carbonate electrolyte has evolved from costly pure lithium carbonate to multicomponent carbonate electrolytes, predominantly based on 10-fold less expensive strontium carbonate. Other advances include the introduction of a new direct cathode press for separation and extraction of the GNC product, as well as specialized modifications of C2CNT for carbon capture, utilization and storage of industrial processes (Genesis CCUS), direct air capture (Genesis DAC) and the separate recovery of the oxygen product (Genesis O2).

Information

Type
Case Study
Creative Commons
Creative Common License - CCCreative Common License - BY
This is an Open Access article, distributed under the terms of the Creative Commons Attribution licence (http://creativecommons.org/licenses/by/4.0), which permits unrestricted re-use, distribution and reproduction, provided the original article is properly cited
Copyright
© The Author(s), 2025. Published by Cambridge University Press
Figure 0

Figure 1. C2CNT decarbonization. (A) The oxide-laden electrolyte of C2CNT is a carbon sink, drawing in CO2 while excluding the other insoluble components of flue gas, such as N2, O2 and H2O. (B) The Genesis CCUS captures CO2 from flue gas without the need to preconcentrate the CO2. The flue gas is separated by a planar insulation membrane from the hot carbon sink electrolyte in the inner electrolysis chamber.

Figure 1

Figure 2. Industrial carbon capture by molten carbonate electrolytic splitting of CO2. (A) The Genesis Device® kiln used for large-scale CO2 molten carbonate electrolysis. (B1 and B2) The cathode, with an active area of 11,000 cm2, upon lifting from the electrolyte and cooling. (C) TGA purity of captured CO2 product measured from multiple carbon capture electrolysis runs in various lithium or mixed strontium/lithium carbonate electrolyte. (D) Carbon nanotube product: SEM and TGA of a 770 °C 60% SrCO3/40 wt% Li2CO3 electrolyte 16-h electrolysis at J = 0.2 A/cm2. (E) Carbon nano-onion product: SEM and TGA of a 770 °C 54% SrCO3, 41% Li2CO3, 5 wt% Na2CO3 electrolyte electrolysis 4-h at J = 0.6 A/cm2.

Figure 2

Figure 3. Extraction, subsequent to CO2 electrolysis: separation of the raw product grown on the cathode from excess electrolyte. (A) A 2021 desktop manual press is used to filter the high-temperature carbanogel raw product into its separate product and electrolyte. (B) A 2024 large-scale hydraulic-driven vertical extraction press. (C) The 2025 industrial CHER extraction unit, designed to repetitively scrape the carbanogel from the electrolysis cathode, separate the GNC product from the excess electrolyte and recover the GNC product made from CO2. (D) The CHER extraction efficiency of removing the electrolyte during repeat post-electrolysis insertion of the raw-product covered cathode.

Figure 3

Figure 4. The direct cathode press electrolyte removal. (A) Illustration of the press and components. (B) Subsequent to electrolysis, the cathode, laden with product and electrolyte (raw product), is moved to the press, as shown in (C), loaded into the press. (D) The cathode is directly pressed (rather than scraped as illustrated in Figure 3), removing electrolyte and retaining the product. (E) The cathode, still retaining the product but with excess electrolyte removed, is lifted from the press. Further details of the direct cathode press, including an action animation and demonstration of actual operation, are provided in the Supplementary Information.

Figure 4

Figure 5. Recent advances in the C2CNT decarbonization process. (A–C) Genesis CCUS: (A) The addition of a porous, insulating membrane above the electrolyte carbon sink thermally isolates the feed gas from the electrolysis. (B) The CO2 diffusion rate through several porous insulation materials. (C) The Genesis CCUS captures CO2 from flue gas without the need to preconcentrate the CO2. (D–F) The Genesis DAC expands the C2CNT process to air as a source of CO2 by expanding the feed gas/electrolysis chamber interfacial membrane for sufficient CO2 diffusion. (G–I) The Genesis O2 configuration separates the CO2 splitting products, facilitating the separate collection of O2 from the anode and carbon nanomaterials from the cathode.

Figure 5

Figure 6. (Top) A commercially operational aluminum smelting plant, illustrating the industrial-scale infrastructure. (Bottom left) Schematic of the current Genesis Device® designed for the electrochemical conversion of 100 tonnes of CO2 per year into graphene nanocarbon (GNC) products such as carbon nanotubes (CNTs). (Bottom right) Conceptual design of a future large-scale Genesis Device system targeting 1 megatonne (Mt) per year of CO2 conversion, producing ~0.25 Mt of GNCs. This scale-up is modeled after aluminum smelting operations and involves a tenfold increase in capacity through the serial integration of kilotonne-per-year (kt/y) Genesis Device modules.

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Author comment: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R0/PR1

Comments

We present for your consideration as a Case Study in Carbon Technology our study entitled:

“Large scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons”

by Gad Licht, Kyle Hofstetter and Stuart Licht.

The study provides significant advances and industrial capabilities of an important decarbonization process for the large scale removal of the greenhouse gas CO2 and its electrochemical spliting to oxygen and useful graphene nanocarbons, such as carbon nanotubes (CNTs). Developments reported in this C2CNT process that will be of interest to your readership in the critical need to mitigate CO2 include industrial scale C2CNT decarbonization design and use, the first reports of capture and utilization of fluegas CO2 as O2 and CNT separate products, a new method for separation of the electrolyte from the high purity CNT product, the use of C2CNT for both carbon utilization and direct air capture processes, and the characterization and applications of the CNTs, made from CO2, in plasmas, polymers composites and buckypaper.

Thank you for your time, efforts and consideration,

Stuart Licht

Professor Emeritus, Department of Chemistry

George Washington University, Washington, DC, USA

Review: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R0/PR2

Conflict of interest statement

Reviewer declares none.

Comments

In this work, the authors present recent advances in molten carbonate electrolysis for the production of carbon-based materials such as graphene nanocarbons (GNCs) and carbon nanotubes (CNTs). The paper provides a detailed description of the process from laboratory scale to pilot-scale demonstrations, supported by experimental data from both small- and large-scale systems. Additionally, the authors explore the impact of CO₂ concentration in the feedstock and describe the recovery processes for carbon and oxygen products.

To provide a broader context, it would be beneficial for the authors to include a discussion on the overall energy balance or energy consumption of the process. For instance, it would be helpful to know the amount of energy required to produce one ton of CNTs or the energy input needed to maintain Li2CO3 in its molten state.

I recommend the authors add commentary on the future challenges of this technology and identify key factors that could enhance CO₂ removal efficiency or improve the overall carbon production process.

Additional minor comments:

• Please ensure consistent formatting of in-text references throughout the manuscript.

• Line 77: Consider specifying the conversion rate or current density at the voltage range of 0.8 to 2 V (e.g., “...energy required for C2CNT electrolysis to convert CO₂ into GNCs ranges from 0.8 to 2 volts (Ren, Lau et al., 2015)...”).

• Line 106: Please clarify whether this should refer to “Figure 1A.”

• Line 158: Double-check the citation formatting for “(Licht, Hofstetter, Licht, Beryllium 2024).”

Review: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R0/PR3

Conflict of interest statement

The reviewer reports no competing interests.

Comments

The authors present a case study providing paths to large-scale carbon capture using molten carbonate electrolysis that splits CO2 into graphene nanocarbons (GNCs). The manuscript is very informative and the details of the technology are very well described, and it is worth publishing from the technical point of view. There are only small technical suggestions. However, the manuscript – as its current form – contains substantial grammar errors and style errors that need to be properly fixed before this work considered for publication. Some of the issues to be fixed are listed below. However, the grammar and presentation errors are not limited to the below list. The authors should carefully revise the manuscript – by referring to the author guideline of Cambridge Prisms – to ensure that the manuscript is free of technical writing and presentation errors. This potentially requires careful proof reading. Some specific comments are listed below:

Technical comments:

Please consider adding a dedicated section that highlights the major advantages of the presented technology versus the other ones. Please also discuss in detail the next steps, scientific milestones, and challenges to be overcome for further improvements. A comparison table could be provided to highlight the major advantages here versus other counterpart technologies.

Non-technical comments to be fixed (not only limited to below – please kindly proof read the manuscript to remove any other errors):

The following sentence appears to be a bit too bold. Please kindly consider smoothing it. “To date all reported CO2 abatement processes have not been demonstrated to be useful or successful on the large scale, and CO2 emissions 17 continue to rise across the planet.”

CNTs should be abbreviated and defined in the first place they appear within the impact statement. The same comment is valid for other abbreviations and definitions.

There needs to be a full stop at the last sentence of the impact statement.

The abstract needs an introductory sentence.

Please kindly revise the following sentence : We’ve developed a large-scale CCUS decarbonization process, We have …

Please kindly correct the punctuation errors in the sentences (coexistence of comma and full stop) on lines 125, 126, 138, 141,

Please kindly correct the grammar error in the sentence on line 181 -> Figures 2D & 2E presents SEM…

Please kindly correct the grammar error in the sentence on line 306 -> Figures 5D - 5F presents t

Please kindly correct the grammar error in the sentence on lines 211-212 -> It is 212 now is scaled up to an industrial …

Please kindly place the relevant references after the sentences on lines 214 and 215.

Please delete the extra space in the bracket on line 234.

Please place a full stop after the sentence on line 244.

Please correct the grammar error on line 252 -> the cathode is .loaded.

Please kindly correct the grammar error on line 277 -> As seen in Figure 5A, e additional N2, O2 and H

In the following sentences, please place the links to the supplementary information and refer them as general information without providing the links inside the manuscript. The Movie 3 259 (https://youtu.be/_UFVd210aec) is a simple animation of the DCP in action, and Movie 4 260 (https://youtu.be/BmbukaCVJko) is a demonstration of the DCP (each is also available in the 261 Supplementary Information).

Please explicitly refer to the figure instead of referring to the previous figure -> this will help readers.

Please kindly correct the presentation of the sentence on line 128 (CO2meter.com sensor). Please present it either in the methods section or within a bracket. The current presentation style is not proper.

Please kindly fix the mixed use of capital and small letters in the sentence (lines 295 and 414) -> 2.5.c Direct Air electrolysis to CO2 to CNTs: Genesis DAC and 414 2.4.e Ongoing applications of CNTs made from CO2 by the C2CNT Process. D

Please correct the grammar error on line 322 -> “ … current is noted, Deviations based on…”

Please correct the grammar error on line 339 -> “ ….. has have several advantages over..”

The panel labelling font size in the figures should be smaller.

Please kindly check the font size and readability of the text in the figures – some fonts are not quite readable and they are not at the same font size with others.

Recommendation: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R0/PR4

Comments

The reviewers recommend two major areas of improvement of the manuscript prior to its acceptance in Cambridge Prisms: Carbon Technologies:

1) The authors should carefully revise the manuscript – by referring to the author guideline of Cambridge Prisms – to ensure that the manuscript is free of technical writing and presentation errors. Many grammatical, formatting, and presentation errors were identified throughout the manuscript which will need to be corrected.

2) The authors should also expand on the overall energy balance/ consumption of the process, as well as provide broader context to the work by including commentary on the future challenges of this technology, identifying key factors that could enhance CO₂ removal efficiency or improve the overall carbon production process/ energy efficiency of the process.

Please review the comments and revise the manuscript to address these points.

Decision: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R0/PR5

Comments

No accompanying comment.

Author comment: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R1/PR6

Comments

Dear Editors,

The Aug. 5 2025 Decision on CAT-2024-001 email Dr. Cao Thang Dinh included revision comments from the Editor and Reviewers that called for grammatical corrections and the additions of two new sections to the manuscript. No mention was made that the manuscript was too long. Each of the corrections, suggestions and addition of the Editor and the Reviewers was fully integrated into the revised manuscript that was uploaded Aug. 8 into the portal. Subsequently, we were contacted Aug. 11 by email by Hannah Gardiner, Carbon Technology Office that the manuscript was around a factor of two too long and that figures must be submitted as separate files. This revision meets those requests. The handling of this manuscript, with information which we feel is urgent and timely to present to the decarbonization community, has taken more than 7 months and we respectfully request its expeditious handling. Thank you, Stuart Licht, Prof. Emeritus, George Washington University

Review: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R1/PR7

Conflict of interest statement

Reviewer declares none.

Comments

The authors have addressed the comments provided in the previous round. I would recommend publication.

Review: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R1/PR8

Conflict of interest statement

Reviewer declares none.

Comments

The author has addressed my concerns.

Recommendation: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R1/PR9

Comments

Thank you for your revision, we are pleased to accept your revised manuscript for publication.

Decision: Large-scale electrolytic molten carbonate carbon capture and transformation to carbon nanotubes and other graphene nanocarbons — R1/PR10

Comments

No accompanying comment.