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Title: A path for lignin valorization via additive manufacturing of high-performance sustainable composites with enhanced 3D printability

Here, we report the manufacture of printable, sustainable polymer systems to address global challenges associated with high-volume utilization of lignin, an industrial waste from biomass feedstock. By analyzing a common three-dimensional printing process—fused-deposition modeling—and correlating the printing-process features to properties of materials such as acrylonitrile-butadiene-styrene (ABS) and nylon, we devised a first-of-its-kind, high-performance class of printable renewable composites containing 40 to 60 weight % (wt %) lignin. An ABS analog made by integrating lignin into nitrile-butadiene rubber needs the presence of a styrenic polymer to avoid filament buckling during printing. However, lignin-modified nylon composites containing 40 to 60 wt % sinapyl alcohol–rich, melt-stable lignin exhibit enhanced stiffness and tensile strength at room temperature, while—unexpectedly—demonstrating a reduced viscosity in the melt. Further, incorporation of 4 to 16 wt % discontinuous carbon fibers enhances mechanical stiffness and printing speed, as the thermal conductivity of the carbon fibers facilitates heat transfer and thinning of the melt. We found that the presence of lignin and carbon fibers retards nylon crystallization, leading to low-melting imperfect crystals that allow good printability at lower temperatures without lignin degradation.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 12; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1489603

Nguyen, Ngoc A., Barnes, Sietske H., Bowland, Christopher C., Meek, Kelly M., Littrell, Kenneth C., Keum, Jong K., and Naskar, Amit K.. A path for lignin valorization via additive manufacturing of high-performance sustainable composites with enhanced 3D printability. United States: N. p., Web. doi:10.1126/sciadv.aat4967.
Nguyen, Ngoc A., Barnes, Sietske H., Bowland, Christopher C., Meek, Kelly M., Littrell, Kenneth C., Keum, Jong K., & Naskar, Amit K.. A path for lignin valorization via additive manufacturing of high-performance sustainable composites with enhanced 3D printability. United States. doi:10.1126/sciadv.aat4967.
Nguyen, Ngoc A., Barnes, Sietske H., Bowland, Christopher C., Meek, Kelly M., Littrell, Kenneth C., Keum, Jong K., and Naskar, Amit K.. 2018. "A path for lignin valorization via additive manufacturing of high-performance sustainable composites with enhanced 3D printability". United States. doi:10.1126/sciadv.aat4967. https://www.osti.gov/servlets/purl/1489603.
@article{osti_1489603,
title = {A path for lignin valorization via additive manufacturing of high-performance sustainable composites with enhanced 3D printability},
author = {Nguyen, Ngoc A. and Barnes, Sietske H. and Bowland, Christopher C. and Meek, Kelly M. and Littrell, Kenneth C. and Keum, Jong K. and Naskar, Amit K.},
abstractNote = {Here, we report the manufacture of printable, sustainable polymer systems to address global challenges associated with high-volume utilization of lignin, an industrial waste from biomass feedstock. By analyzing a common three-dimensional printing process—fused-deposition modeling—and correlating the printing-process features to properties of materials such as acrylonitrile-butadiene-styrene (ABS) and nylon, we devised a first-of-its-kind, high-performance class of printable renewable composites containing 40 to 60 weight % (wt %) lignin. An ABS analog made by integrating lignin into nitrile-butadiene rubber needs the presence of a styrenic polymer to avoid filament buckling during printing. However, lignin-modified nylon composites containing 40 to 60 wt % sinapyl alcohol–rich, melt-stable lignin exhibit enhanced stiffness and tensile strength at room temperature, while—unexpectedly—demonstrating a reduced viscosity in the melt. Further, incorporation of 4 to 16 wt % discontinuous carbon fibers enhances mechanical stiffness and printing speed, as the thermal conductivity of the carbon fibers facilitates heat transfer and thinning of the melt. We found that the presence of lignin and carbon fibers retards nylon crystallization, leading to low-melting imperfect crystals that allow good printability at lower temperatures without lignin degradation.},
doi = {10.1126/sciadv.aat4967},
journal = {Science Advances},
number = 12,
volume = 4,
place = {United States},
year = {2018},
month = {12}
}

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