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1. Lignin Nanoparticles and Alginate Gel Beads: Preparation, Characterization and Removal of Methylene Blue

   https://doi.org/10.3390/nano12010176  

   Luo, Tong; Hao, Yanping; Wang, Chao; Jiang, Weikun; Ji, Xingxiang; Yang, Guihua; Chen, Jiachuan; Janaswamy, Srinivas; Lyu, Gaojin (January 2022, Nanomaterials)

   A novel and effective green system consisting of deep eutectic solvent (DES) was proposed to prepare lignin nanoparticles (LNPs) without any lignin modification. The LNPs are obtained through the dialysis of the kraft lignin-DES solution. The particle size distribution, Zeta potential and morphology of the LNPs are characterized by using dynamic light scattering (DLS), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The average diameter of LNPs is in the range 123.6 to 140.7 nm, and the LNPs show good stability and dispersibility in water. The composite beads composed of LNPs and sodium alginate (SA) are highly efficient (97.1%) at removing methylene blue (MB) from the aqueous solution compared to 82.9% and 77.4% by the SA/bulk kraft lignin composite and pure SA, respectively. Overall, the LNPs-SA bio-nanocomposite with high adsorption capacity (258.5 mg/g) could be useful in improving water quality and other related applications. 

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2. In Vivo Toxicity Assessment of Chitosan-Coated Lignin Nanoparticles in Embryonic Zebrafish (Danio rerio)

   https://doi.org/10.3390/nano11010111  

   Stine, Jared S.; Harper, Bryan J.; Conner, Cathryn G.; Velev, Orlin D.; Harper, Stacey L. (January 2021, Nanomaterials)

   null (Ed.)

   Lignin is the second most abundant biopolymer on Earth after cellulose. Since lignin breaks down in the environment naturally, lignin nanoparticles may serve as biodegradable carriers of biocidal actives with minimal environmental footprint compared to conventional antimicrobial formulations. Here, a lignin nanoparticle (LNP) coated with chitosan was engineered. Previous studies show both lignin and chitosan to exhibit antimicrobial properties. Another study showed that adding a chitosan coating can improve the adsorption of LNPs to biological samples by electrostatic adherence to oppositely charged surfaces. Our objective was to determine if these engineered particles would elicit toxicological responses, utilizing embryonic zebrafish toxicity assays. Zebrafish were exposed to nanoparticles with an intact chorionic membrane and with the chorion enzymatically removed to allow for direct contact of particles with the developing embryo. Both mortality and sublethal endpoints were analyzed. Mortality rates were significantly greater for chitosan-coated LNPs (Ch-LNPs) compared to plain LNPs and control groups. Significant sublethal endpoints were observed in groups exposed to Ch-LNPs with chorionic membranes intact. Our study indicated that engineered Ch-LNP formulations at high concentrations were more toxic than plain LNPs. Further study is warranted to fully understand the mechanisms of Ch-LNP toxicity. 

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3. Engineered Sorghum Bagasse Enables a Sustainable Biorefinery with p ‐Hydroxybenzoic Acid‐Based Deep Eutectic Solvent

   https://doi.org/10.1002/cssc.202101492  

   Wang, Yunxuan; Meng, Xianzhi; Tian, Yang; Kim, Kwang_Ho; Jia, Linjing; Pu, Yunqiao; Leem, Gyu; Kumar, Deepak; Eudes, Aymerick; Ragauskas, Arthur_J; et al (October 2021, ChemSusChem)

   Abstract Integrating multidisciplinary research in plant genetic engineering and renewable deep eutectic solvents (DESs) can facilitate a sustainable and economic biorefinery. Herein, we leveraged a plant genetic engineering approach to specifically incorporate C₆C₁monomers into the lignin structure. By expressing the bacterialubiCgene in sorghum,p‐hydroxybenzoic acid (PB)‐rich lignin was incorporated into the plant cell wall while this monomer was completely absent in the lignin of the wild‐type (WT) biomass. A DES was synthesized with choline chloride (ChCl) and PB and applied to the pretreatment of the PB‐rich mutant biomass for a sustainable biorefinery. The release of fermentable sugars was significantly enhanced (∼190 % increase) compared to untreated biomass by the DES pretreatment. In particular, the glucose released from the pretreated mutant biomass was up to 12 % higher than that from the pretreated WT biomass. Lignin was effectively removed from the biomass with the preservation of more than half of the β‐Ο‐4 linkages without condensed aromatic structures. Hydrogenolysis of the fractionated lignin was conducted to demonstrate the potential of phenolic compound production. In addition, a simple hydrothermal treatment could selectively extract PB from the same engineered lignin, showing a possible circular biorefinery. These results suggest that the combination of PB‐based DES and engineered PB‐rich biomass is a promising strategy to achieve a sustainable closed‐loop biorefinery. 

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4. Scalable Formation of Concentrated Monodisperse Lignin Nanoparticles by Recirculation‐Enhanced Flash Nanoprecipitation

   https://doi.org/10.1002/ppsc.202000122  

   Conner, Cathryn G.; Veleva, Anka N.; Paunov, Vesselin N.; Stoyanov, Simeon D.; Velev, Orlin D. (June 2020, Particle & Particle Systems Characterization)

   Abstract A highly controllable and scalable process for fabrication of large amounts of concentrated lignin nanoparticles (LNPs) is reported. These lignin core nanoparticles are formed through flash nanoprecipitation, however, scaling up of the fabrication process requires fundamental understanding of their operational formation mechanism and surface properties. It is shown how a semicontinuous synthesis system with a recirculation loop makes it possible to produce flash precipitated lignin nanoparticles in large amounts for practical applications. The roles of the process parameters, including flow rates and lignin concentration, are investigated and analyzed. The results indicate that the LNPs are formed by a process of continuous burst nucleation at the point of mixing without diffusive growth, which yields nanoparticles of highly uniform size following a modified LaMer nucleation and growth mechanism. This mechanism makes possible facile process control and scale‐up. Effective control of the resulting nanoparticle size is achieved through the initial concentration of lignin in the injected solution. The impressive capability to produce suspensions of any predesigned multimodal distribution is demonstrated. The resulting nanofabrication technique can produce large volumes of concentrated LNP suspensions of high stability and tightly controlled size distributions for biological or agricultural applications. 

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5. Experimental Thermal Conductivity Studies of Agar-Based Aqueous Suspensions with Lignin Magnetic Nanocomposites

   https://doi.org/10.3390/magnetochemistry10020012  

   Gautam, Bishal; Nabat_Al-Ajrash, Saja M; Hasan, Mohammad Jahid; Saini, Abhishek; Watzman, Sarah J; Ureña-Benavides, Esteban; Vasquez-Guardado, Erick S (February 2024, Magnetochemistry)

   Nanoparticle additives increase the thermal conductivity of conventional heat transfer fluids at low concentrations, which leads to improved heat transfer fluids and processes. This study investigates lignin-coated magnetic nanocomposites (lignin@Fe3O4) as a novel bio-based magnetic nanoparticle additive to enhance the thermal conductivity of aqueous-based fluids. Kraft lignin was used to encapsulate the Fe3O4 nanoparticles to prevent agglomeration and oxidation of the magnetic nanoparticles. Lignin@Fe3O4 nanoparticles were prepared using a pH-driven co-precipitation method with a 3:1 lignin to magnetite ratio and characterized by X-ray diffraction, FT-IR, thermogravimetric analysis, and transmission electron microscopy. The magnetic properties were characterized using a vibrating sample magnetometer. Once fully characterized, lignin@Fe3O4 nanoparticles were dispersed in aqueous 0.1% w/v agar–water solutions at five different concentrations, from 0.001% w/v to 0.005% w/v. Thermal conductivity measurements were performed using the transient line heat source method at various temperatures. A maximum enhancement of 10% in thermal conductivity was achieved after adding 0.005% w/v lignin@Fe3O4 to the agar-based aqueous suspension at 45 °C. At room temperature (25 °C), the thermal conductivity of lignin@Fe3O4 and uncoated Fe3O4 agar-based suspensions was characterized at varying magnetic fields from 0 to 0.04 T, which were generated using a permanent magnet. For this analysis, the thermal conductivity of lignin magnetic nanosuspensions initially increased, showing a 5% maximum peak increase after applying a 0.02 T magnetic field, followed by a decreasing thermal conductivity at higher magnetic fields up to 0.04 T. This result is attributed to induced magnetic nanoparticle aggregation under external applied magnetic fields. Overall, this work demonstrates that lignin-coated Fe3O4 nanosuspension at low concentrations slightly increases the thermal conductivity of agar aqueous-based solutions, using a simple permanent magnet at room temperature or by adjusting temperature without any externally applied magnetic field. 

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