Structural and molecular-weight-dependency in the formation of lignin nanoparticles from fractionated soft- and hardwood lignins

Pylypchuk, Ievgen V.; Riazanova, Anastasia V.; Lindström, Mikael; Sevastyanova, Olena

doi:10.1039/d0gc04058d

Cited by 78 publications

(68 citation statements)

References 46 publications

(67 reference statements)

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“…TEM results correlated closest to the number distribution from light scattering. 1 As it has been already shown in previous studies (Lievonen et al, 2016;Pylypchuk et al, 2021), the size of LNPs is usually proportional to the pre-dialysis lignin concentrations. However, using the acetone-insoluble fraction of lignin (fraction N5), the LNP size was shown to be independent of initial pre-dialysis lignin concentrations (Figure 2B).…”

Section: Resultsmentioning

confidence: 81%

High-Molecular-Weight Fractions of Spruce and Eucalyptus Lignin as a Perspective Nanoparticle-Based Platform for a Therapy Delivery in Liver Cancer

Pylypchuk

Suo

Chucheepchuenkamol

et al. 2022

Front. Bioeng. Biotechnol.

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The natural polymer, lignin, possesses unique biodegradable and biocompatible properties, making it highly attractive for the generation of nanoparticles for targeted cancer therapy. In this study, we investigated spruce and eucalyptus lignin nanoparticles (designated as S-and E-LNPs, respectively). Both LNP types were generated from high-molecular-weight (Mw) kraft lignin obtained as insoluble residues after a five-step solvent fractionation approach, which included ethyl acetate, ethanol, methanol, and acetone. The resulting S-and E-LNPs ranged in size from 16 to 60 nm with uniform spherical shape regardless of the type of lignin. The preparation of LNPs from an acetone-insoluble lignin fraction is attractive because of the use of high-Mw lignin that is otherwise not suitable for most polymeric applications, its potential scalability, and the consistent size of the LNPs, which was independent of increased lignin concentrations. Due to the potential of LNPs to serve as delivery platforms in liver cancer treatment, we tested, for the first time, the efficacy of newly generated E-LNPs and S-LNPs in two types of primary liver cancer, hepatocellular carcinoma (HCC) and cholangiocarcinoma (CCA), in vitro. Both S-LNPs and E-LNPs inhibited the proliferation of HCC cells in a dose-dependent manner and did not affect CCA cell line growth. The inhibitory effect toward HCC was more pronounced in the E-LNP-treated group and was comparable to the standard therapy, sorafenib. Also, E-LNPs induced late apoptosis and necroptosis while inhibiting the HCC cell line. This study demonstrated that an elevated number of carbohydrates on the surface of the LNPs, as shown by NMR, seem to play an important role in mediating the interaction between LNPs and eukaryotic cells. The latter effect was most pronounced in E-LNPs. The novel S- and E-LNPs generated in this work are promising materials for biomedicine with advantageous properties such as small particle size and tailored surface functionality, making them an attractive and potentially biodegradable delivery tool for combination therapy in liver cancer, which still has to be verified in vivo using HCC and CCA models.

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Section: Resultsmentioning

confidence: 81%

High-Molecular-Weight Fractions of Spruce and Eucalyptus Lignin as a Perspective Nanoparticle-Based Platform for a Therapy Delivery in Liver Cancer

Pylypchuk

Suo

Chucheepchuenkamol

et al. 2022

Front. Bioeng. Biotechnol.

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“…[ 7 , 8 , 9 , 10 , 11 , 12 , 13 ] The ongoing paradigm shift towards lignin‐based advanced engineered materials is largely based on the superior properties of lignin nanoparticles (LNPs), which have emerged as a thriving research field in recent years. [ 7 , 14 , 15 , 16 , 17 ]…”

Section: Introductionmentioning

confidence: 99%

Unravelling the Hydration Barrier of Lignin Oleate Nanoparticles for Acid‐ and Base‐Catalyzed Functionalization in Dispersion State

et al. 2021

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Lignin nanoparticles (LNPs) are promising renewable nanomaterials with applications ranging from biomedicine to water purification. However, the instability of LNPs under acidic and basic conditions severely limits their functionalization for improved performance. Here, we show that controlling the degree of esterification can significantly improve the stability of lignin oleate nanoparticles (OLNPs) in acidic and basic aqueous dispersions. The high stability of OLNPs is attributed to the alkyl chains accumulated in the shell of the particle, which delays protonation/deprotonation of carboxylic acid and phenolic hydroxyl groups. Owing to the enhanced stability, acid‐ and base‐catalyzed functionalization of OLNPs at pH 2.0 and pH 12.0 via oxirane ring‐opening reactions were successfully performed. We also demonstrated these new functionalized particles as efficient pH‐switchable dye adsorbents and anticorrosive particulate coatings.

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“…We know that SKL is a heterogeneous and polydisperse material composed of branched amphiphilic molecules [47] . Carboxylic acid and phenolic hydroxyl groups are enriched in the low molecular weight fraction that constitutes the charged shell of OLNPs [16, 48] . Building on these facts, a hypothesis can be set forth that the amphiphilic lignin oleate molecules orient so that their carboxylic groups are exposed to the water phase surrounding the particles.…”

Section: Resultsmentioning

confidence: 99%

“…However, lignin is currently largely destined for combustion, representing a missed opportunity for functional nanomaterials [7–13] . The ongoing paradigm shift towards lignin‐based advanced engineered materials is largely based on the superior properties of lignin nanoparticles (LNPs), which have emerged as a thriving research field in recent years [7, 14–17] …”

Section: Introductionmentioning

confidence: 99%

“…[7][8][9][10][11][12][13] Theo ngoing paradigm shift towards lignin-based advanced engineered materials is largely based on the superior properties of lignin nanoparticles (LNPs), which have emerged as at hriving research field in recent years. [7,[14][15][16][17] In contrast to bulk lignin, LNPs resist aggregation in aqueous dispersions (pH 3-9) owing to their sub-micrometer size and electrostatic repulsion between ionized carboxylic acid groups on their surfaces. [17] This anionic surface charge together with aw ell-defined spherical shape and al arge surface area to mass ratio make them viable candidates for physical modification via adsorption of positively charged compounds such as enzymes or polymers.…”

Section: Introductionmentioning

confidence: 99%

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Unravelling the Hydration Barrier of Lignin Oleate Nanoparticles for Acid‐ and Base‐Catalyzed Functionalization in Dispersion State

et al. 2021

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Structural and molecular-weight-dependency in the formation of lignin nanoparticles from fractionated soft- and hardwood lignins

Abstract: The use of lignin from forests as a renewable resource is a greener alternative to the petrochemical industry and accelerates the progress towards the development of more environmentally friendly industrial...

Cited by 78 publications

References 46 publications

High-Molecular-Weight Fractions of Spruce and Eucalyptus Lignin as a Perspective Nanoparticle-Based Platform for a Therapy Delivery in Liver Cancer

High-Molecular-Weight Fractions of Spruce and Eucalyptus Lignin as a Perspective Nanoparticle-Based Platform for a Therapy Delivery in Liver Cancer

Unravelling the Hydration Barrier of Lignin Oleate Nanoparticles for Acid‐ and Base‐Catalyzed Functionalization in Dispersion State

Unravelling the Hydration Barrier of Lignin Oleate Nanoparticles for Acid‐ and Base‐Catalyzed Functionalization in Dispersion State

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