Carbon capture in polymer-based electrolytes

Author:

Wang Yang1ORCID,Feric Tony G.23ORCID,Tang Jing145ORCID,Fang Chao16ORCID,Hamilton Sara T.37ORCID,Halat David M.16ORCID,Wu Bing1ORCID,Celik Hasan8ORCID,Rim Guanhe37ORCID,DuBridge Tara1,Oshiro Julianne1ORCID,Wang Rui16ORCID,Park Ah-Hyung Alissa237ORCID,Reimer Jeffrey A.167ORCID

Affiliation:

1. Department of Chemical and Biomolecular Engineering, College of Chemistry, UC Berkeley, Berkeley, CA 94720, USA.

2. Department of Chemical Engineering, Columbia University, New York, NY 10027, USA.

3. Lenfest Center for Sustainable Energy, Columbia University, New York, NY 10027, USA.

4. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, USA.

5. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.

6. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

7. Department of Earth and Environmental Engineering, Columbia University, New York, NY 10027, USA.

8. College of Chemistry Nuclear Magnetic Resonance Facility (CoC-NMR), University of California, Berkeley, CA 94720, USA.

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.

Publisher

American Association for the Advancement of Science (AAAS)

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