Engineering Papers⌕ Search
Home/Archive/DOE OSTI

DOE OSTI · 3384982

Solvent-Mediated Control of Nanocellulose Dispersion: An Integrated Computational and Experimental Investigation

Yu, Yan [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics]·Rukmani, Shalini J. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0000000184749403)·Wan, Zhangmin [Univ. of British Columbia, Vancouver, BC (Canada)] (ORCID:0000000311780308)·Copenhaver, Katie [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000322618760)·Goswami, Monojoy [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000244734888)·Li, Kai [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000314453206)·Ozcan, Soydan [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000238254589)·Rojas, Orlando J. [Univ. of British Columbia, Vancouver, BC (Canada)] (ORCID:0000000340364020)·Smith, Jeremy C. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0000000229783227)
View original source ↗Read source document ↗Export metadata ↓

Abstract

Fibrillated cellulose derived from forestry feedstocks represents a renewable and high-strength materials platform for circular bioeconomies. However, its practical implementation is hindered by the irreversible aggregation of nanocellulose architectures, including cellulose nanofibers (CNFs). Solvent-based dispersion offers a simple and practical route to prevent CNF aggregation. Here, in this work, we integrate classical and enhanced sampling molecular dynamics (MD) simulations with experimental suspension rheology and atomic force microscopy (AFM) to elucidate how solvent environments tune CNF–CNF interactions and dispersion stability. CNF–CNF contact free energies computed from MD simulations reveal reduced aggregation in acetone/water, γ-valerolactone (GVL)/water, and tetrahydrofuran (THF)/water and pure acetone compared with pure water, reflecting stronger CNF-solvent relative to inter-CNF interactions. Correspondingly, CNF-solvent suspensions in these solvent systems exhibit stronger inter-fibril network structures and enhanced recovery compared to water, indicating improved CNF-solvent affinity. Liquid cell AFM imaging in acetone–water mixtures and in pure acetone further confirm the presence of well-dispersed CNFs. By combining multiscale computation with targeted experiments, this study establishes a rational framework for solvent design to achieve stable nanocellulose dispersions for high-strength biobased materials and efficient bioenergy conversion.

Explore related subjects

cellulosecomputer simulationsnanofiberssolventsthermodynamic properties

Keep this discovery

BibTeXRIS

Yu, Yan [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics], Rukmani, Shalini J. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0000000184749403), Wan, Zhangmin [Univ. of British Columbia, Vancouver, BC (Canada)] (ORCID:0000000311780308), Copenhaver, Katie [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000322618760), Goswami, Monojoy [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000244734888), Li, Kai [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000314453206), Ozcan, Soydan [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000238254589), Rojas, Orlando J. [Univ. of British Columbia, Vancouver, BC (Canada)] (ORCID:0000000340364020), Smith, Jeremy C. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0000000229783227). 2026-06-22. Solvent-Mediated Control of Nanocellulose Dispersion: An Integrated Computational and Experimental Investigation. https://doi.org/10.1021/acsnano.6c06855

Cite the original work for its findings. Save a collection to share your selection of sources.

Discover connections

cellulose subjectcomputer simulations subjectnanofibers subjectsolvents subjectthermodynamic properties subject

Connections use source metadata and explicit phrase matches, not verified experimental comparisons.

KEEP EXPLORING

Related reports

DOE OSTI2026

Hybrid Bio-Based Composites: Enabling Cellulose Nanofiber (CNF) Incorporation into Composites via Macroscale Natural Fiber Carriers

Cellulose nanofibers (CNFs) have significant potential in composites as additives to improve mechanical properties, melt rheology, and more. However, agglomeration of CNFs is a key challenge in composite melt processing as obtaining nano-level dispersion of CNFs often requires cost- and energy-intensive processes (e.g., solvent exchange or freeze drying) due to the strong hornification tendencies of CNF. Herein, we avoid these challenges by using a natural fiber carrier method to integrate CNF into thermoplastic composites. Fibers are co-dried to create a hybrid fiber feedstock for compounding in which natural fibers are decorated with dispersed nanofibers. The hybridized fibers result in up to a 24% increase in tensile strength and up to a 35% increase in Young’s modulus compared to composites only containing natural fibers. The lignocellulosic nanofibers are found to outperform their purely cellulosic counterpart, which is theorized to be due to either an increased propensity for fibrillation of the lignocellulosic fibers or the increased hydrophobicity of the fibers due to the presence of lignin. Surface analysis of fiber feedstocks, via streaming potential measurements and dynamic light scattering (DLS), confirmed a significant change in the feedstock hydrophobicity before and after hybridization. While mild additions of CNF (1 wt.% on the macroscale fiber) do not impact the composite melt viscosity, the viscosity is found to increase at higher CNF loadings (5 wt.% on the macroscale fiber), indicating its utility as a rheology modifier. Lastly, use of these materials as novel feedstocks for medium-scale additive manufacturing in high-fidelity part production was demonstrated.

bio-based↗
DOE OSTI2023

Polymer grafted aramid nanofiber reinforces immiscible waste polypropylene/poly(ethylene terephthalate)

Polypropylene (PP) and poly(ethylene terephthalate) (PET) are plastics commonly used for packaging because of their excellent barrier and mechanical properties. The properties of these plastics are often diminished after mechanical recycling, inevitably causing down-cycling. Furthermore, this problem is exacerbated when different kinds of polymers mix. Aramid nanofibers have the potential to improve the mechanical properties of polymers due to their excellent mechanical properties but their poor dispersion in polymers is a challenge. Grafting polymers onto nanofibers can help address this challenge. In this work, different loading levels (1%, 2%, and 5%) of polymer grafted aramid nanofibers (ANFs) are blended with waste PP/PET (90/10), simulating a PP waste stream containing traces of PET contaminants. Scanning electronic microscopy, rheology, and differential scanning calorimetry results show the affinity of PP functionalized aramid nanofibers (PP_ANF) towards the PP matrix. At 1 wt% of the nanofiber, the size of the PET droplets in the PP matrix of the PP_ANF blend range from 0.2 to 2.0 μm while that of unmodified ANF and PET_ANF blends are in the range of 0.1–6.2 and 0.5–7.4 μm, respectively. In summary, polymer grafted ANFs have the tendency of improving properties of its like polymers due to similarity in the grafting polymer and the polymer matrix.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Synthesis and application of thermally responsive nanofiber coatings for overtemperature monitoring

This study presents a one-pot synthesis route to organometallic nanofibers based on copper thiolate, exhibiting distinctive chemical and physical characteristics. Electron microscopy analysis of morphology and composition revealed 2-10 μm-long, 50-90 nm-diameter hollow and non-hollow fibers composed of copper, sulfur, oxygen, hydrocarbon, and chlorine. Thermogravimetric analysis showed a pronounced mass loss within 120°C-135°C. To elucidate the thermal responsive pathways, the nanofibers were characterized before and after heating. X-ray photoelectron spectroscopy indicates that an initially mixed Cu(I)/Cu(II) oxidation states transition to predominantly Cu(I) upon heating. A layer of nanofiber was coated on battery pouch foil and evaluated as a candidate thermally sensitive coating. At elevated temperature (100-130°C), nanofiber coating released volatile organic compounds, sulfide and sulfur dioxide as detected using multiple gas sensors. This thermally responsive gas release/sensing approach provides a potential large-area temperature monitoring strategy, which is particularly relevant where direct temperature measurements of individual batteries is impractical. The results established proof of concept for nanofiber-coated battery pouch foil as overtemperature warning platform that can provide alerts when surface temperatures exceed a critical threshold. More broadly, the ability to form interconnected fiber networks positions copper thiolate nanofiber coatings as promising materials for advanced applications.

Ihala Gamaralalage, Chanaka [ORNL] (ORCID:00000002↗