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

Abstract

Materials made from renewable resources are interesting 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 discuss, 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 windowmore » of entangled concentration (4–6.5 wt%) of biomass in the IL was determined to be favorable for fiber spinning.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office
OSTI Identifier:
1557507
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Green Chemistry
Additional Journal Information:
Journal Volume: 21; Journal Issue: 16; Journal ID: ISSN 1463-9262
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Nguyen, Ngoc A., Kim, Keonhee, Bowland, Christopher C., Keum, Jong K., Kearney, Logan T., André, Nicolas, Labbé, Nicole, and Naskar, Amit K. A fundamental understanding of whole biomass dissolution in ionic liquid for regeneration of fiber by solution-spinning. United States: N. p., 2019. Web. doi:10.1039/C9GC00774A.
Nguyen, Ngoc A., Kim, Keonhee, Bowland, Christopher C., Keum, Jong K., Kearney, Logan T., André, Nicolas, Labbé, Nicole, & Naskar, Amit K. A fundamental understanding of whole biomass dissolution in ionic liquid for regeneration of fiber by solution-spinning. United States. doi:10.1039/C9GC00774A.
Nguyen, Ngoc A., Kim, Keonhee, Bowland, Christopher C., Keum, Jong K., Kearney, Logan T., André, Nicolas, Labbé, Nicole, and Naskar, Amit K. Thu . "A fundamental understanding of whole biomass dissolution in ionic liquid for regeneration of fiber by solution-spinning". United States. doi:10.1039/C9GC00774A. https://www.osti.gov/servlets/purl/1557507.
@article{osti_1557507,
title = {A fundamental understanding of whole biomass dissolution in ionic liquid for regeneration of fiber by solution-spinning},
author = {Nguyen, Ngoc A. and Kim, Keonhee and Bowland, Christopher C. and Keum, Jong K. and Kearney, Logan T. and André, Nicolas and Labbé, Nicole and Naskar, Amit K.},
abstractNote = {Materials made from renewable resources are interesting 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 discuss, 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.},
doi = {10.1039/C9GC00774A},
journal = {Green Chemistry},
number = 16,
volume = 21,
place = {United States},
year = {2019},
month = {6}
}

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