A fundamental understanding of whole biomass dissolution in ionic liquid for regeneration of fiber by solution-spinning

Ngoc A. Nguyen, Keonhee Kim, Christopher C. Bowland, Jong K. Keum, Logan T. Kearney, Nicolas André, Nicole Labbé, Amit K. Naskar

Research output: Contribution to journalArticlepeer-review

30 Scopus citations

Abstract

Materials generated from renewable resources are promising and attractive substitutes for petroleum-based materials. Recently, regeneration of cellulose fibers using ionic liquids (ILs) as green solvents has been a topic of interest to both industrial and academic sectors. However, extraction of cellulose from lignocellulosic biomass requires numerous energy intensive processing steps. Additionally, the deconstruction and removal of lignin and hemicellulose components from lignocellulosic biomass usually involve corrosive pretreatment and the solvation of specific biomass components. Instead, utilization of the whole biomass - particularly woody residues - to manufacture high-performance materials offers an attractive value-proposition. In this study, we demonstrated fiber regeneration of whole hybrid poplar (HP) biomass by a sustainable method. We developed an environmentally friendly approach by partially auto-hydrolyzing the biomass with water before its dissolution in 1-ethyl-3-methylimidazolium acetate ([C2mim][OAc]) ionic liquid, for large-scale, roll-to-roll production of fibers by solution spinning. We report, for the first time, a fundamental understanding of the inter- and intramolecular interactions in HP biomass-IL solutions, as well as their corresponding spinnability, structural reformation, and mechanical performance of the regenerated fibers. Particularly, the molecular alignment, recrystallization, and crystallinity of the spun fibers were correlated to the chain entanglement, molecular relaxation, and rheological properties of the HP biomass-IL solutions. A window of entangled concentration (4-6.5 wt%) of biomass in the IL was determined to be favorable for fiber spinning.

Original languageEnglish
Pages (from-to)4354-4367
Number of pages14
JournalGreen Chemistry
Volume21
Issue number16
DOIs
StatePublished - 2019

Funding

This research at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the US Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy, BioEnergy Technologies Office Program. J.K.K acknowledges the DOE Office of Science User Facility through the Center for Nanophase Materials Sciences, the Oak Ridge National Laboratory. N. L. acknowledges the Research Council of Norway (BioMim project) for partial funding. We thank Austin X. Staub and Jedidiah L. Long for assistance with the mechanical testing. This manuscript has been 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).

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