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

Title: Carbon capture in polymer-based electrolytes

Journal Article · 19 April 2024 · Science Advances

DOI: https://doi.org/10.1126/sciadv.adk2350 · OSTI ID:2396809

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Univ. of California, Berkeley, CA (United States); SLAC
Columbia Univ., New York, NY (United States)
Univ. of California, Berkeley, CA (United States); Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Columbia Univ., New York, NY (United States)

Nanoparticle organic hybrid materials (NOHMs) have been proposed as excellent electrolytes for combined CO₂ capture and electrochemical conversion due to their conductive nature and chemical tunability. However, CO₂ capture behavior and transport properties of these electrolytes after CO₂ 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 CO₂ capture. Quantitative ¹³C NMR spectra collected at variable temperatures reveal that absorbed CO₂ exists as carbamates (RHNCOO^– or RR'NCOO^–) and carbonate/bicarbonate (CO₃^2–/HCO₃^–). The transport properties of PEI and NOHM-I-PEI studied using ¹H 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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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2396809

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 16 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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