Abstract
Liquid-like nanoparticle organic hybrid materials (NOHMs) consisting of a silica core with ionically grafted branched polyethyleneimine chains (referred to as NIPEI) are encapsulated within submicron-scale polyacrylonitrile (PAN)/polymer-derived-ceramic electrospun fibers. The addition of a room-temperature curable, liquid-phase organopolysilazane (OPSZ) ceramic precursor to the PAN/NOHM solution enhances the internal dispersion of NOHMs and forms a thin ceramic sheath layer on the fiber exterior, shielding the hydrophilic NIPEI to produce near-superhydrophobic non-woven fiber mats with contact angles exceeding 140°. 60:40 loadings of NOHMs to PAN/OPSZ can be reliably achieved with low OPSZ percentages required, and up to 4:1 NOHM:polymer loadings are possible before losing hydrophobicity. These fibers demonstrate up to ≈2 mmol CO2 g−1 fiber capture capacities in a pure CO2 atmosphere through the nonwoven fibrous networks and the permeability of the OPSZ shell. The hybrid fibers additionally show enhanced capture kinetics under pure CO2 and 400 ppm CO2 conditions, indicating their promising application as a direct air capture platform.
| Original language | English |
|---|---|
| Article number | 2301649 |
| Journal | Advanced Functional Materials |
| Volume | 33 |
| Issue number | 32 |
| DOIs | |
| State | Published - Aug 8 2023 |
Funding
K.D.K. performed all electrospinning work and microscopy, porometry, and contact angle characterization for the polymer fibers in this study. CO capture tests were performed by G.H.L., J.H.X., and M.K.K. TGA analysis to determine the NIPEI loadings was performed by M.K.K. and G.H.L. NIPEI was synthesized by G.H.L. The manuscript was written by K.D.K., with the CO capture methods and TGA methods sections provided by G.H.L. and M.K.K. Conceptualization and project supervision at Cornell was done by Y.L.J., while project supervision at ORNL and Columbia was carried out by M.K.K and A.‐H.A.P., respectively. The authors acknowledge the funding for this work provided by the Office of Fossil Energy Carbon Managment in the U.S. Department of Energy (DE‐FE0031963 and FWP 3FEAA392). This work also made use of the Cornell Center for Materials Research Shared Facilities, which were supported through the NSF MRSEC program (DMR‐1719875). Notice: This manuscript was authored by UT‐Battelle, LLC, under contract DE‐AC05‐00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid‐up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe‐public‐access‐plan ). 2 2 K.D.K. performed all electrospinning work and microscopy, porometry, and contact angle characterization for the polymer fibers in this study. CO2 capture tests were performed by G.H.L., J.H.X., and M.K.K. TGA analysis to determine the NIPEI loadings was performed by M.K.K. and G.H.L. NIPEI was synthesized by G.H.L. The manuscript was written by K.D.K., with the CO2 capture methods and TGA methods sections provided by G.H.L. and M.K.K. Conceptualization and project supervision at Cornell was done by Y.L.J., while project supervision at ORNL and Columbia was carried out by M.K.K and A.-H.A.P., respectively. The authors acknowledge the funding for this work provided by the Office of Fossil Energy Carbon Managment in the U.S. Department of Energy (DE-FE0031963 and FWP 3FEAA392). This work also made use of the Cornell Center for Materials Research Shared Facilities, which were supported through the NSF MRSEC program (DMR-1719875). Notice: This manuscript was authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).
Keywords
- CO capture
- direct air capture
- gas-assisted electrospinning
- nanoparticle organic hybrid materials
- polymer-ceramic hybrid fibers
- selective water rejection