Carbon capture in polymer-based electrolytes

Wang, Yang; Feric, Tony G.; Tang, Jing; Fang, Chao; Hamilton, Sara T.; Halat, David M.; Wu, Bing; Celik, Hasan; Rim, Guanhe; DuBridge, Tara; Oshiro, Julianne; Wang, Rui; Park, Ah-Hyung Alissa; Reimer, Jeffrey A.

doi:10.1126/sciadv.adk2350

DOE OSTI · 2396809

Carbon capture in polymer-based electrolytes

Wang, Yang·Feric, Tony G.·Tang, Jing·Fang, Chao·Hamilton, Sara T.·Halat, David M.·Wu, Bing·Celik, Hasan·Rim, Guanhe·DuBridge, Tara·Oshiro, Julianne·Wang, Rui·Park, Ah-Hyung Alissa·Reimer, Jeffrey A.

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Abstract

Nanoparticle organic hybrid materials (NOHMs) have been proposed as excellent electrolytes for combined CO 2 capture and electrochemical conversion due to their conductive nature and chemical tunability. However, CO 2 capture behavior and transport properties of these electrolytes after CO 2 capture have not yet been studied. Here, we use a variety of nuclear magnetic resonance (NMR) techniques to explore the carbon speciation and transport properties of branched polyethylenimine (PEI) and PEI-grafted silica nanoparticles (denoted as NOHM-I-PEI) after CO 2 capture. Quantitative 13 C NMR spectra collected at variable temperatures reveal that absorbed CO 2 exists as carbamates (RHNCOO – or RR'NCOO – ) and carbonate/bicarbonate (CO 3 2– /HCO 3 – ). The transport properties of PEI and NOHM-I-PEI studied using 1 H pulsed-field-gradient NMR, combined with molecular dynamics simulations, demonstrate that coulombic interactions between negatively and positively charged chains dominate in PEI, while the self-diffusion in NOHM-I-PEI is dominated by silica nanoparticles. These results provide strategies for selecting adsorbed forms of carbon for electrochemical reduction.

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Wang, Yang, Feric, Tony G., Tang, Jing, Fang, Chao, Hamilton, Sara T., Halat, David M., Wu, Bing, Celik, Hasan, Rim, Guanhe, DuBridge, Tara, Oshiro, Julianne, Wang, Rui, Park, Ah-Hyung Alissa, Reimer, Jeffrey A.. 2024-04-19. Carbon capture in polymer-based electrolytes. https://doi.org/10.1126/sciadv.adk2350

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