R-014

Vladislav Ivaništšev [a,d]

vladislav.ivanistsev@ut.ee

Iuliia Vetik [a], Nikita Žoglo [b], Akmal Kosimov [a], Ritums Cepitis [a], Veera Krasnenko [c], Vitali Grozovski [a], Nadezda Kongi [a]

[a] Institute of Chemistry, University of Tartu, Tartu 50411, Estonia

[b] RedoxNRG OÜ, Narva-Jõesuu 29021, Estonia

[c] Institute of Physics, University of Tartu, Tartu 50411, Estonia 

[d] Department of Chemistry, University of Latvia, Jelgavas iela 1, LV-1004 Riga, Latvia

Electrochemical CO2 capture with metal-organic frameworks

The criteria for viability of CO2 capture include operability in ambient conditions, stability, and scalability. Most importantly is to minimize the energy required for reversible capture and release of CO2, below the deployment cost of 100 $ per ton of CO2 [1] (Fig. 1).

We introduce the first metal-organic framework (MOF) that captures and releases CO2 under ambient aqueous electrochemical conditions [2]. Copper-2,3,6,7,10,11- hexahydroxy- triphenylene Cu3(HHTP)2 operates reversibly at standard temperature, pressure, and in open air. Beyond performance, it demonstrates a new electrosorption mechanism with a partial transfer coupled with the CO2 adsorption. Its combinatorial 3-in-1 composition means wider space for improvement than previously in case of known sorbents. Such space is suitable for searching electrosorbents with as high efficiency as needed to meet the above defined viability criteria (Fig. 1).

In this presentation, we focus on the mechanism of adsorption in Cu3(HHTP)2-like MOFs with variable pore size using the density functional theory simulations (Fig. 1). The process was validated experimentally with cyclic voltammetry and differential electrochemical mass spectrometry [2]. New computational insights show that the electrochemical parameters – potential, capacity, and adsorption energy – of the CO2 capture–release process can be tuned based on an atomistic-level understanding of the electrosorption mechanism (Fig 1). We report results highlight the potential of conductive MOFs with built-in redox and structural versatility as tunable electrosorbents suitable for direct-air and -ocean capture.

Acknowledgements: This presentation is supported by the Estonian Ministry of Education and Research (TK210) and the Estonian Research Council (grant STP52)

References: 

[1] Negative Emissions Technologies and Reliable Sequestration: A Research Agenda, The National Academies Press, Washington, DC, 2019. https://doi.org/10.17226/25259. 

[2] I. Vetik, N. Žoglo, A. Kosimov, R. Cepitis, V. Krasnenko, H. Qing, P. Chandra, K. Mirica, R. Rizo, E. Herrero, J. Solla-Gullón, T. Trisukhon, J.W. Gittins, A.C. Forse, V. Grozovski, N. Kongi, V. Ivaništšev, Advancing Electrochemical CO2 Capture with Redox-Active Metal-Organic Frameworks, (2024). https://doi.org/10.48550/arXiv.2411.16444.