Copolymerizing Lignin for Tuned Properties of 3D-Printed PEG-Based Photopolymers

Ruiz Deance, Ana Laura; Siersema, Bjorn; Yoe, Laurine Eleonora Anne-Catherine; Wurm, Frederik R.; Gojzewski, Hubert

doi:10.1021/acsapm.3c01875

Cited by 3 publications

(1 citation statement)

References 71 publications

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“…[ 5d,7 ] However, when spherical nanoobjects such as lignin nanospheres are encapsulated in the photoresins, the scattering effect can be amplified. [ 6c,9 ] This is ascribed to the nano‐effect with limited light penetration and the discrepancy in the refractive index between lignin nanospheres and the crosslinked hydrogel network, which results in an incomplete‐curing effect. Commonly, the amphiphilic nature of the lignin macromolecule is prone to supporting the formation of spherical lignin nanoparticles in its self‐assembly driven by the solubility change when processed from a soluble form to nano‐lignin.…”

Section: Introductionmentioning

confidence: 99%

Evolution of Self‐Assembled Lignin Nanostructure into Dendritic Fiber in Aqueous Biphasic Photocurable Resin for DLP‐Printing

Wang,

Wu,

Wang

et al. 2024

Adv Funct Materials

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The design of lignin nanostructures where interfacial interactions enable enhanced entanglement of colloidal networks can broaden their applications in hydrogel‐based materials and light‐based 3D printing. Herein, an approach for fabricating surface‐active dendritic colloidal microparticles (DCMs) characterized by fibrous structures using nanostructured allylated lignin is proposed for the development of lignin‐based photocurable resins. With allyl‐terminated surface functionality of 0.61 mmol g−1, the entanglement between lignin‐DCM fibrils with a size of 1.4 µm successfully produces only lignin‐based hydrogels with structural integrity through photo‐crosslinking. The colloidal network of lignin dendricolloids reinforces the poly(ethylene glycol) (PEG) hydrogels during a digital light processing (DLP) 3D printing process by generating bicontinuous morphologies, resulting in six‐fold increases in toughness values with respect to the neat PEG hydrogel. The dual effectiveness of photoabsorption and free‐radical reactivity of lignin‐DCMs allow the light‐patterning of rather dilute PEG hydrogels (5–10%) with high geometric fidelity and structural complexity via DLP 3D printing. This study demonstrates a green and effective strategy for the design of 1D lignin‐DCMs that increases the versatility of the nanostructured biopolymer, opening up numerous opportunities for formulating functional hydrogels with robust structure‐property correlations.

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Section: Introductionmentioning

confidence: 99%

Evolution of Self‐Assembled Lignin Nanostructure into Dendritic Fiber in Aqueous Biphasic Photocurable Resin for DLP‐Printing

Wang,

Wu,

Wang

et al. 2024

Adv Funct Materials

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Decolorization of Lignin for High‐Resolution 3D Printing of High Lignin‐Content Composites

Böcherer,

Montazeri,

et al. 2024

Advanced Science

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Lignin, one of the most abundant biomaterials and a large‐scale industrial waste product, is a promising filler for polymers as it reduces the amount of fossil resources and is readily available. 3D printing is well‐known for producing detailed polymer structures in small sizes at low waste production. Especially light‐assisted 3D printing is a powerful technique for production of high‐resolution structures. However, lignin acts as a very efficient absorber for UV and visible light limiting the printability of lignin composites, reducing its potential as a high‐volume filler. In this work, the decolorization of lignin is presented for high‐resolution 3D printing of biocomposites with lignin content up to 40 wt.%. Organosolv lignin (OSL) is decolorized by an optimized low‐energy process of acetylation and subsequent UV irradiation reducing the UV absorbance by 71%. By integration of decolorized lignin into bio‐based tetrahydrofurfuryl acrylate (THFA), a lignin content of 40 wt.% and a resolution of 250 µm is achieved. Due to the reinforcing properties of lignin, the stiffness and strength of the material is increased by factors of 15 and 2.3, respectively. This work paves the way for the re‐use of a large amount of lignin waste for 3D printing of tough materials at high resolution.

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Biobased Flame-Retardant Polylactic Acid Foams through Lignin-Based Nanocarriers Encapsulating Deoxyribonucleic Acid

Ridard,

Duvigneau,

Mayer-Gall

et al. 2024

ACS Sustainable Chem. Eng.

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Lignin-based nanocarriers loaded with deoxyribonucleic acid (DNA) are investigated as a potential biobased flame-retardant additive in polylactic acid (PLA). The progressive ban of halogenatedbased flame retardant has pushed toward developing more benign alternatives like phosphorus-containing biomaterials. DNA is thus of interest, since it is a biobased and abundant source of phosphates containing synergistic nitrogen and aromatic units in its structure. Here, we report the use of DNA to prepare biobased and flameretardant PLA foams, which might be used for lightweight packaging or building insulation. For the first time, DNA was successfully encapsulated in lignin-based nanocarriers in situ via cross-linking in an inverse miniemulsion. Surface-grafting of the lignin nanocarriers (LNCs) with OH-terminated PLA is conducted to enhance the compatibility in the PLA matrix during the following composite preparation and adjustment of the LNC amounts from 1 to 20 wt %. Pressurized CO 2 allows foaming the PLA composites, indicating that LNCs are promoting nucleation, leading to smaller cells and lighter foams even at low loading (1 wt %) compared to neat PLA, making them efficient biobased nucleating agents. Thermal stability of the PLA nanocomposites was reduced systematically when LNCs were added up to ca. 50 °C compared to neat PLA, and the flame retardant properties show an expected trend, i.e., the more DNA is introduced, the lower total heat release is observed. The LOI values of the foams, ranging from 25 to 30, are higher compared to those of their respective unfoamed composites. Overall, this strategy shows the potential of biopolymers to enhance flame retardancy of bioplastics and avoid toxic polymer additives.

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Copolymerizing Lignin for Tuned Properties of 3D-Printed PEG-Based Photopolymers

Cited by 3 publications

References 71 publications

Evolution of Self‐Assembled Lignin Nanostructure into Dendritic Fiber in Aqueous Biphasic Photocurable Resin for DLP‐Printing

Evolution of Self‐Assembled Lignin Nanostructure into Dendritic Fiber in Aqueous Biphasic Photocurable Resin for DLP‐Printing

Decolorization of Lignin for High‐Resolution 3D Printing of High Lignin‐Content Composites

Biobased Flame-Retardant Polylactic Acid Foams through Lignin-Based Nanocarriers Encapsulating Deoxyribonucleic Acid

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