<i>In Situ</i> NMR Spectroscopy of Nanoconfined Aqueous Electrolyte and CO ₂ for Carbon Capture and Energy Storage

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🔬研究者:This study provides novel NMR methodologies and mechanistic insights into nanoconfined electrolyte behavior for supercapacitor-based carbon capture.

🏢実務担当者:The findings could inform the design of dual-use supercapacitors for CO2 capture and energy storage in industrial settings.

Aqueous electrolyte supercapacitors are investigated for their applications in CO 2 capture[1] and in energy storage.[2] These devices use microporous carbon electrodes with aqueous electrolyte, and can be capacitively charged through formation of an electrochemical double layer inside the microporous electrode structure. Charging stores energy and leads to reversible uptake of CO 2 from an external gas reservoir. These devices use cheap and safe materials, are extremely stable to repeated cycling, and possess dual-use functionality; however, their use is limited by relatively lower energy storage performance and CO 2 capacity than equivalent devices. Additionally, further optimisation of these devices towards industrial deployment is limited by 1) the unclear mechanism of capacitive charging, particularly in regards to the role of pH; 2) the unclear mechanism of CO 2 capture; 3) uncertainties around aqueous chemistry in nanoconfinement. In this work, we demonstrate a variety of in situ nuclear magnetic resonance (NMR) spectroscopy techniques for probing behaviour of nanoconfined aqueous electrolyte inside electrodes: Magic-angle-spinning 1 H and 13 C NMR spectroscopy allows measurement of speciation of water, electrolyte ions, and CO 2 into different physical environments (e.g. in-pore vs ex-pore) and different chemical environments (e.g. CO 2 vs. HCO 3 - ) inside electrodes; NMR exchange spectroscopy enables quantitative measurement of exchange between these different chemical and physical environments; Application of NMR probe molecules allows for characterisation of aqueous chemistry under nanoconfinement. Through these techniques, we identify significant changes in CO 2 dissolution in nanoconfined electrolyte compared to bulk electrolyte,[3] changes in speciation upon altering electrolyte pH which correlate with changing electrochemical behaviour,[4] and changes in the in-pore aqueous chemistry upon charging the activated carbon electrode. These insights provide significant insight into how species behave inside nanoconfined electrolyte, and demonstrate the applicability of in situ NMR techniques for similar studies across other energy storage, separation, and catalytic systems. References [1] Khan, F. ulHaq; Bilal, M.; Li, J.; Xu, X.; Landskron, K. Supercapacitive Swing Adsorption of CO 2 : Advances and Future Prospects. Trends in Chemistry 2025, 7 (1), 43–55. [2] Bragg, R. J.; Griffiths, K.; Hwang, I.; Leketas, M.; Polus, K.; Presser, V.; Dryfe, R. A. W.; Griffin, J. M. Solvation Effects on Aqueous Ion Adsorption and Electrosorption in Carbon Micropores. Carbon 2024, 229, 119531. [3] Coady, Z.; Brookes, S. G. H.; Shen, Z.; Rhodes, B. J.; Mapstone, G.; Xu, Z.; Yu, W.; Nishihara, H.; Schran, C.; Michaelides, A.; Forse, A. C. Unexpected Oversolubility of CO 2 Measured at Electrode–Electrolyte Interfaces. J. Am. Chem. Soc. 2025. [4] Wiesner, S. E.; Coady, Z.; Xu, Z.; Forse, A. Supercapacitor-Based CO 2 Capture Enhanced by Electrolyte pH Control. ChemRxiv.

• openalex https://doi.org/10.1149/ma2026-01552626mtgabsfirst seen 2026-07-18 05:43:26