Additive Manufacturing with Cellulose-Based Composites: Materials, Modeling, and Applications

De, Shuvodeep; Rukmani, Shalini J.; Zhao, Xianhui; Clarkson, Caitlyn; Vautard, Frederic; Bhagia, Samarthya; Goswami, Monojoy; Zhang, Shuyang; Elyas, Sana F.; Zhao, Wei; Smith, Jeremy C.; Ragauskas, Arthur J.; Ozcan, Soydan; Tekinalp, Halil; Si, Muqing; Huang, Jinrui; He, Ximin

doi:10.1002/adfm.202414222

Additive Manufacturing with Cellulose-Based Composites: Materials, Modeling, and Applications

Journal Article · Sun Dec 29 23:00:00 EST 2024 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202414222· OSTI ID:2502181

^[1]; ^[2]; ^[1]; ^[1]; Vautard, Frederic ^[1]; Bhagia, Samarthya ^[1]; ^[1]; Zhang, Shuyang ^[3]; Elyas, Sana F. ^[1]; Zhao, Wei ^[4]; ^[5]; ^[6]; ^[1]; Tekinalp, Halil ^[1]; Si, Muqing ^[7]; Huang, Jinrui ^[7]; ^[7]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oklahoma State Univ., Stillwater, OK (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Molecular Biophysics
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Univ. of California, Los Angeles, CA (United States)

Recent advances in large-scale additive manufacturing (AM) with polymer-based composites have enabled efficient production of high-performance materials. Cellulose nanomaterials (CNMs) have emerged as bio-based feedstocks due to their exceptional strength and sustainability. However, challenges such as hornification and poor dispersion in polymer matrices still limit large-scale CNM–polymer composite manufacturing, requiring novel strategies. Here, this review outlines an approach starting with atomic-level simulations to link molecular composition to key parameters like bulk density, viscosity, and modulus. These simulations provide data for finite element analysis (FEA), which informs large-scale experiments and reduces the need for extensive trials. The strategy explores how atomic interactions impact the morphology, adhesion, and mechanical properties of CNM-based composites in AM processes. The review also discusses current developments in AM, along with predictions of mechanical and thermal properties for structural applications, packaging, flexible electronics, and hydrogel scaffolds. By integrating experimental findings with molecular dynamics (MD) simulations and finite element modeling (FEM), valuable insights for material design, process optimization, and performance enhancement in CNM-based AM are provided to address ongoing challenges.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Bioenergy Technologies Office (BETO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2502181

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 7 Vol. 35; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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3D printing of a recycled copolyester of terephthalic acid, cyclohexanedimethanol and tetramethylcyclobutanediol Bhagia, Samarthya; Kore, Surbhi; Wasti, Sanjita Polymer Testing, Vol. 118 https://doi.org/10.1016/j.polymertesting.2022.107916	journal	January 2023
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Loose Pre-Cross-Linking Mediating Cellulose Self-Assembly for 3D Printing Strong and Tough Biomimetic Scaffolds Guo, Jinhua; Li, Qingtao; Zhang, Rongrong Biomacromolecules, Vol. 23, Issue 3 https://doi.org/10.1021/acs.biomac.1c01330	journal	February 2022
3D Bioprinting Human Chondrocytes with Nanocellulose–Alginate Bioink for Cartilage Tissue Engineering Applications Markstedt, Kajsa; Mantas, Athanasios; Tournier, Ivan Biomacromolecules, Vol. 16, Issue 5 https://doi.org/10.1021/acs.biomac.5b00188	journal	April 2015
Using COSMO-RS to Predict Hansen Solubility Parameters Wojeicchowski, José Pedro; Ferreira, Ana M.; Okura, Tifany Industrial & Engineering Chemistry Research, Vol. 61, Issue 42 https://doi.org/10.1021/acs.iecr.2c01592	journal	July 2022
Use of Microfibrillated Cellulose/Lignosulfonate Blends as Carbon Precursors: Impact of Hydrogel Rheology on 3D Printing Shao, Ying; Chaussy, Didier; Grosseau, Philippe Industrial & Engineering Chemistry Research, Vol. 54, Issue 43 https://doi.org/10.1021/acs.iecr.5b02763	journal	October 2015
Development of a New Coarse-Grained Model to Simulate Assembly of Cellulose Chains Due to Hydrogen Bonding Wu, Zijie; Beltran-Villegas, Daniel J.; Jayaraman, Arthi Journal of Chemical Theory and Computation, Vol. 16, Issue 7 https://doi.org/10.1021/acs.jctc.0c00225	journal	June 2020
New Patchy Particle Model with Anisotropic Patches for Molecular Dynamics Simulations: Application to a Coarse-Grained Model of Cellulose Nanocrystal Rolland, Nicolas; Mehandzhiyski, Aleksandar Y.; Garg, Mohit Journal of Chemical Theory and Computation, Vol. 16, Issue 6 https://doi.org/10.1021/acs.jctc.0c00259	journal	May 2020
Extending the Martini 3 Coarse-Grained Force Field to Carbohydrates Lutsyk, Valery; Wolski, Pawel; Plazinski, Wojciech Journal of Chemical Theory and Computation, Vol. 18, Issue 8 https://doi.org/10.1021/acs.jctc.2c00553	journal	July 2022
Martini 3 Coarse-Grained Force Field for Carbohydrates Grünewald, Fabian; Punt, Mats H.; Jefferys, Elizabeth E. Journal of Chemical Theory and Computation, Vol. 18, Issue 12 https://doi.org/10.1021/acs.jctc.2c00757	journal	November 2022
Water as an Intrinsic Structural Element in Cellulose Fibril Aggregates Chen, Pan; Wohlert, Jakob; Berglund, Lars The Journal of Physical Chemistry Letters, Vol. 13, Issue 24 https://doi.org/10.1021/acs.jpclett.2c00781	journal	June 2022
A Combined Theoretical and Experimental Study of the Polymer Matrix-Mediated Stress Transfer in a Cellulose Nanocomposite Peterson, Anna; Mehandzhiyski, Aleksandar Y.; Svenningsson, Leo Macromolecules, Vol. 54, Issue 7 https://doi.org/10.1021/acs.macromol.0c02305	journal	March 2021
Achieving Enhanced Interfacial Adhesion and Dispersion in Cellulose Nanocomposites via Amorphous Interfaces Xia, Wenjie; Qin, Xin; Zhang, Yao Macromolecules, Vol. 51, Issue 24 https://doi.org/10.1021/acs.macromol.8b02243	journal	December 2018
Quantifying Localized Macromolecular Dynamics within Hydrated Cellulose Fibril Aggregates Chen, Pan; Terenzi, Camilla; Furó, István Macromolecules, Vol. 52, Issue 19 https://doi.org/10.1021/acs.macromol.9b00472	journal	September 2019
Tuning Glass Transition in Polymer Nanocomposites with Functionalized Cellulose Nanocrystals through Nanoconfinement Qin, Xin; Xia, Wenjie; Sinko, Robert Nano Letters, Vol. 15, Issue 10 https://doi.org/10.1021/acs.nanolett.5b02588	journal	September 2015
Tuning the Nanotopography and Chemical Functionality of 3D Printed Scaffolds through Cellulose Nanocrystal Coatings Babi, Mouhanad; Riesco, Roberto; Boyer, Louisa ACS Applied Bio Materials, Vol. 4, Issue 12 https://doi.org/10.1021/acsabm.1c00970	journal	November 2021
Poplar as Biofiber Reinforcement in Composites for Large-Scale 3D Printing Zhao, Xianhui; Tekinalp, Halil; Meng, Xianzhi ACS Applied Bio Materials, Vol. 2, Issue 10 https://doi.org/10.1021/acsabm.9b00675	journal	August 2019
Volumetric Double-Layer Charge Storage in Composites Based on Conducting Polymer PEDOT and Cellulose Sahalianov, Ihor; Say, Mehmet Girayhan; Abdullaeva, Oliya S. ACS Applied Energy Materials, Vol. 4, Issue 8 https://doi.org/10.1021/acsaem.1c01850	journal	August 2021
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Matrix-Assisted Three-Dimensional Printing of Cellulose Nanofibers for Paper Microfluidics Shin, Sungchul; Hyun, Jinho ACS Applied Materials & Interfaces, Vol. 9, Issue 31 https://doi.org/10.1021/acsami.7b07609	journal	July 2017
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Direct Cryo Writing of Aerogels Via 3D Printing of Aligned Cellulose Nanocrystals Inspired by the Plant Cell Wall Kam, Doron; Chasnitsky, Michael; Nowogrodski, Chen Colloids and Interfaces, Vol. 3, Issue 2 https://doi.org/10.3390/colloids3020046	journal	April 2019
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Cellulose Nanofibrils Filled Poly(Lactic Acid) Biocomposite Filament for FDM 3D Printing Wang, Qianqian; Ji, Chencheng; Sun, Lushan Molecules, Vol. 25, Issue 10 https://doi.org/10.3390/molecules25102319	journal	May 2020
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Perspectives on the Lindman Hypothesis and Cellulose Interactions Norgren, Magnus; Costa, Carolina; Alves, Luís Molecules, Vol. 28, Issue 10 https://doi.org/10.3390/molecules28104216	journal	May 2023
Cellulose Nanocrystals vs. Cellulose Nanofibers: A Comparative Study of Reinforcing Effects in UV-Cured Vegetable Oil Nanocomposites Barkane, Anda; Kampe, Edgars; Platnieks, Oskars Nanomaterials, Vol. 11, Issue 7 https://doi.org/10.3390/nano11071791	journal	July 2021
DLP 3D Printing Meets Lignocellulosic Biopolymers: Carboxymethyl Cellulose Inks for 3D Biocompatible Hydrogels Melilli, Giuseppe; Carmagnola, Irene; Tonda-Turo, Chiara Polymers, Vol. 12, Issue 8 https://doi.org/10.3390/polym12081655	journal	July 2020
3D Printed Polycaprolactone/Gelatin/Bacterial Cellulose/Hydroxyapatite Composite Scaffold for Bone Tissue Engineering Cakmak, Abdullah M.; Unal, Semra; Sahin, Ali Polymers, Vol. 12, Issue 9 https://doi.org/10.3390/polym12091962	journal	August 2020
Finite Element Analysis of Gas Diffusion in Polymer Nanocomposite Systems Containing Rod-like Nanofillers Htira, Thouaiba; Zid, Sarra; Zinet, Matthieu Polymers, Vol. 13, Issue 16 https://doi.org/10.3390/polym13162615	journal	August 2021
Effect of Biomass as Nucleating Agents on Crystallization Behavior of Polylactic Acid Shi, Kang; Liu, Guoshuai; Sun, Hui Polymers, Vol. 14, Issue 20 https://doi.org/10.3390/polym14204305	journal	October 2022
Preparation of 3D Printed Polylactic Acid/Bacterial Cellulose Composite Scaffold for Tissue Engineering Applications Wu, Yadong; Wang, Yunfeng; Wang, Fang Polymers, Vol. 14, Issue 21 https://doi.org/10.3390/polym14214756	journal	November 2022
Enhancing the Mechanical Properties of 3D-Printed Waterborne Polyurethane-Urea and Cellulose Nanocrystal Scaffolds through Crosslinking Vadillo, Julen; Larraza, Izaskun; Calvo-Correas, Tamara Polymers, Vol. 14, Issue 22 https://doi.org/10.3390/polym14224999	journal	November 2022
Poly(lactic acid) and Nanocrystalline Cellulose Methacrylated Particles for Preparation of Cryogelated and 3D-Printed Scaffolds for Tissue Engineering Leonovich, Mariia; Korzhikov-Vlakh, Viktor; Lavrentieva, Antonina Polymers, Vol. 15, Issue 3 https://doi.org/10.3390/polym15030651	journal	January 2023
A Review of Cellulose Coarse-Grained Models and Their Applications Mehandzhiyski, Aleksandar Y.; Zozoulenko, Igor Polysaccharides, Vol. 2, Issue 2 https://doi.org/10.3390/polysaccharides2020018	journal	April 2021

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MICRO-CELLULOSE FIBER REINFORCED BIOCOMPOSITES FOR ADDITIVE MANUFACTURING

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36 MATERIALS SCIENCE
additive manufacturing
composites
fibrillation
finite element modeling
molecular dynamics
nanocellulose

Additive Manufacturing with Cellulose-Based Composites: Materials, Modeling, and Applications

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