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Title: High modulus biocomposites via additive manufacturing: Cellulose nanofibril networks as “microsponges”

Abstract

For the successful transition of additive manufacturing (AM) from prototyping to manufacturing of structural load bearing parts, feedstock systems with improved mechanical properties are needed. In terms of sustainability and environmental impact, selection of biobased renewable alternatives instead of petroleum-based options is important. Nanocellulose, which gives plants and trees their structural integrity, can offer significant improvements in the mechanical properties of AM polymers, provided that the right fibril morphology, dispersion and adhesion are achieved. In this study, although the interfacial adhesion between the hydrophilic cellulose nanofibrils (CNFs) and the hydrophobic polylactate matrix was not strong, and the optimal dispersion in individual fibril level was not attained, dramatic improvements in mechanical properties of neat polymer were achieved (up to 80% tensile strength increase, up to 200% elastic modulus increase). An interlocking reinforcing mechanism in which CNF bundles act as “microsponges” was proposed and supported by high resolution electron microscopy images, x-ray computed chromatography scans and thermal and dynamic mechanical behavior. Additively manufactured samples showed significantly higher elastic modulus (7.12 GPa vs. 6.57 GPa at 30 wt % CNF content) and dramatically improved storage modulus (1.72 GPa vs. 0.9 GPa at 30 wt % CNF content) in the printing direction compared tomore » compression molded samples. Finally, in conclusion, preparation and 3D-printing of a 100% biobased renewable feedstock material with substantial mechanical property improvements were successfully demonstrated, which can open up new window of opportunities in the AM industry.« less

Authors:
 [1]; ORCiD logo [2];  [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. ORNL; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. ORNL; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. ORNL; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Manufacturing Demonstration Facility
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1528739
Alternate Identifier(s):
OSTI ID: 1556791
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Composites Part B: Engineering
Additional Journal Information:
Journal Volume: 173; Journal Issue: C; Journal ID: ISSN 1359-8368
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; A.Composites; A.Nano-cellulose fibres; B.Microstructures; A.Poly(lactic acid); E.Additive manufacturing

Citation Formats

Tekinalp, Halil L., Meng, Xiangtao, Lu, Yuan, Kunc, Vlastimil, Love, Lonnie, Peter, William, and Ozcan, Soydan. High modulus biocomposites via additive manufacturing: Cellulose nanofibril networks as “microsponges”. United States: N. p., 2019. Web. doi:10.1016/j.compositesb.2019.05.028.
Tekinalp, Halil L., Meng, Xiangtao, Lu, Yuan, Kunc, Vlastimil, Love, Lonnie, Peter, William, & Ozcan, Soydan. High modulus biocomposites via additive manufacturing: Cellulose nanofibril networks as “microsponges”. United States. https://doi.org/10.1016/j.compositesb.2019.05.028
Tekinalp, Halil L., Meng, Xiangtao, Lu, Yuan, Kunc, Vlastimil, Love, Lonnie, Peter, William, and Ozcan, Soydan. Sun . "High modulus biocomposites via additive manufacturing: Cellulose nanofibril networks as “microsponges”". United States. https://doi.org/10.1016/j.compositesb.2019.05.028. https://www.osti.gov/servlets/purl/1528739.
@article{osti_1528739,
title = {High modulus biocomposites via additive manufacturing: Cellulose nanofibril networks as “microsponges”},
author = {Tekinalp, Halil L. and Meng, Xiangtao and Lu, Yuan and Kunc, Vlastimil and Love, Lonnie and Peter, William and Ozcan, Soydan},
abstractNote = {For the successful transition of additive manufacturing (AM) from prototyping to manufacturing of structural load bearing parts, feedstock systems with improved mechanical properties are needed. In terms of sustainability and environmental impact, selection of biobased renewable alternatives instead of petroleum-based options is important. Nanocellulose, which gives plants and trees their structural integrity, can offer significant improvements in the mechanical properties of AM polymers, provided that the right fibril morphology, dispersion and adhesion are achieved. In this study, although the interfacial adhesion between the hydrophilic cellulose nanofibrils (CNFs) and the hydrophobic polylactate matrix was not strong, and the optimal dispersion in individual fibril level was not attained, dramatic improvements in mechanical properties of neat polymer were achieved (up to 80% tensile strength increase, up to 200% elastic modulus increase). An interlocking reinforcing mechanism in which CNF bundles act as “microsponges” was proposed and supported by high resolution electron microscopy images, x-ray computed chromatography scans and thermal and dynamic mechanical behavior. Additively manufactured samples showed significantly higher elastic modulus (7.12 GPa vs. 6.57 GPa at 30 wt % CNF content) and dramatically improved storage modulus (1.72 GPa vs. 0.9 GPa at 30 wt % CNF content) in the printing direction compared to compression molded samples. Finally, in conclusion, preparation and 3D-printing of a 100% biobased renewable feedstock material with substantial mechanical property improvements were successfully demonstrated, which can open up new window of opportunities in the AM industry.},
doi = {10.1016/j.compositesb.2019.05.028},
journal = {Composites Part B: Engineering},
number = C,
volume = 173,
place = {United States},
year = {Sun Sep 01 00:00:00 EDT 2019},
month = {Sun Sep 01 00:00:00 EDT 2019}
}

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Works referenced in this record:

The importance of carbon fiber to polymer additive manufacturing
journal, September 2014

  • Love, Lonnie J.; Kunc, Vlastamil; Rios, Orlando
  • Journal of Materials Research, Vol. 29, Issue 17
  • DOI: 10.1557/jmr.2014.212

Tensile and thermomechanical properties of short carbon fiber reinforced polyamide 6 composites
journal, August 2013


Mechanical behavior of carbon fiber reinforced polyamide composites
journal, October 2003


Measurement and analytical validation of interfacial bond strength of PAN-fiber-reinforced carbon matrix composites
journal, March 2008


Influence of thermal history on the mechanical properties of carbon fiber–acrylate composites cured by electron beam and thermal processes
journal, February 2013


Highly oriented carbon fiber–polymer composites via additive manufacturing
journal, December 2014


A study of the mechanical properties of short natural-fiber reinforced composites
journal, December 2005


On the use of nanocellulose as reinforcement in polymer matrix composites
journal, December 2014


Natural fiber polymer composites: A review
journal, January 1999


A review on the tensile properties of natural fiber reinforced polymer composites
journal, June 2011


Hemp Fiber-Reinforced 1-Pentene/Polypropylene Copolymer: The Effect of Fiber Loading on the Mechanical and Thermal Characteristics of the Composites
journal, September 2008

  • Khoathane, M. C.; Vorster, O. C.; Sadiku, E. R.
  • Journal of Reinforced Plastics and Composites, Vol. 27, Issue 14
  • DOI: 10.1177/0731684407086325

The Path Forward for Biofuels and Biomaterials
journal, January 2006

  • Ragauskas, Arthur J.; Williams, Charlotte K.; Davison, Brian H.
  • Science, Vol. 311, Issue 5760, p. 484-489
  • DOI: 10.1126/science.1114736

Nanocellulose in polymer composites and biomedical applications
journal, July 2014

  • Lu, Yuan; Tekinalp, Halil Levent; Eberle, Claude Clifford
  • TAPPI Journal, Vol. 13, Issue 6
  • DOI: 10.32964/TJ13.6.47

A cellulose nanocrystal-based composite electrolyte with superior dimensional stability for alkaline fuel cell membranes
journal, January 2015

  • Lu, Yuan; Armentrout, Aaron A.; Li, Juchuan
  • Journal of Materials Chemistry A, Vol. 3, Issue 25
  • DOI: 10.1039/C5TA02304A

Short fiber reinforced composites for fused deposition modeling
journal, March 2001


Nanofiber-reinforced polymers prepared by fused deposition modeling: Nanofiber-Reinforced Polymers
journal, June 2003

  • Shofner, M. L.; Lozano, K.; Rodríguez-Macías, F. J.
  • Journal of Applied Polymer Science, Vol. 89, Issue 11
  • DOI: 10.1002/app.12496

Cellulose nanofibril (CNF) reinforced starch insulating foams
journal, September 2014


Surface Engineering of Ultrafine Cellulose Nanofibrils toward Polymer Nanocomposite Materials
journal, April 2013

  • Fujisawa, Shuji; Saito, Tsuguyuki; Kimura, Satoshi
  • Biomacromolecules, Vol. 14, Issue 5
  • DOI: 10.1021/bm400178m

The effect of crystallization of PLA on the thermal and mechanical properties of microfibrillated cellulose-reinforced PLA composites
journal, June 2009


Characterization of residual stress and deformation in additively manufactured ABS polymer and composite specimens
journal, September 2017


Tensile properties of short-glass-fiber- and short-carbon-fiber-reinforced polypropylene composites
journal, October 2000


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Vegetable Additives in Food Packaging Polymeric Materials
journal, December 2019