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Artificial muscle materials promise incredible applications in actuators, robotics and medical apparatus, yet the ability to mimic the full characteristics of skeletal muscles into synthetic materials remains a huge challenge. Herein, inspired by the dynamic sacrificial bonds in biomaterials and the self-strengthening of skeletal muscles by physical exercise, high performance artificial muscle material is prepared by rearrangement of sacrificial coordination bonds in the polyolefin elastomer via a repetitive mechanical training process. Biomass lignin is incorporated as a green reinforcer for the construction of interfacial coordination bonds. The prepared artificial muscle material exhibits high actuation strain (>40%), high actuation stress (1.5 MPa) which can lift more than 10,000 times its own weight with 30% strain, characteristics of excellent self-strengthening by mechanical training, strain-adaptive stiffening, and heat/electric programmable actuation performance. In this work, we show a facile strategy for the fabrication of intelligent materials using easily available raw materials. Artificial muscles have a wide range of applications yet truly mimetic designs remain a challenge. Here, the authors use dynamic sacrificial bonds which are rearranged via a mechanical training process to optimise the characteristics of self-strengthening, strain-adaptive stiffening and actuation.

Thought-out utilization of entire lignocellulose is of great importance to achieving sustainable and cost-effective biorefineries. However, there is a trade-off between efficient carbohydrate utilization and lignin-to-chemical conversion yield. Here, we fractionate corn stover into a carbohydrate fraction with high enzymatic digestibility and reactive lignin with satisfactory catalytic depolymerization activity using a mild high-solid process with aqueous diethylamine (DEA). During the fractionation, in situ amination of lignin achieves extensive delignification, effective lignin stabilization, and dramatically reduced nonproductive adsorption of cellulase on the substrate. Furthermore, by designing a tandem fractionation-hydrogenolysis strategy, the dissolved lignin is depolymerized and aminated simultaneously to co-produce monophenolics and pyridine bases. The process represents the viable scheme of transforming real lignin into pyridine bases in high yield, resulting from the reactions between cleaved lignin side chains and amines. This work opens a promising approach to the efficient valorization of lignocellulose. Utilization of the entire lignocellulose is essential for sustainable and cost-effective biorefineries, but it is hindered by a trade-off between efficient carbohydrate utilization and lignin-to-chemical conversion yield. Here, the authors report a mild lignocellulosic fractionation process using aqueous diethylamine which produces a carbohydrate fraction susceptible to enzymatic hydrolysis and a high-quality lignin that delivers high monomer yields upon catalytic amination and depolymerization.

Pickering emulsion stabilized by lignin/sodium dodecyl sulfate composite nanoparticles (LSNP) was used as template to prepare the avermectin @ lignin/polyurea composite microcapsules (AVM@LPMC) through ion cross-linking and interfacial polymerization. The inner wall of the microcapsules is a firm and compact polyurea layer, and the outer wall is a loose lignin layer. The effects of stirring speed, dosage of sodium dodecyl sulfate (SDS), and pH value in aqueous phase on the formation of microcapsules were systematically studied. The results showed that the optimal stirring speed was 200 rpm, and the optimal dosage ratio in water phase was HCl (mmol):SDS (mmol):lignin AL (g) = 0.375:1.25:1 in fixed oil-water ratio (1:9) and oil phase composition. In this way, the encapsulation efficiency of microcapsules could reach up to 85.4%, while it would slightly decrease with the increase of lignin content in the wall materials. The polyurea layer played a key role in supporting the spherical structure of the capsule wall and delaying the release of avermectin, while the loose lignin layer contributed less to the slow release performance of microcapsule. By changing the amount of lignin, the polyurea-layer thickness could be regulated to adjust the release rate of microcapsule. Remarkably, a small amount of lignin introduced in the wall material could significantly improve the anti-photolysis performance of avermectin in microcapsules.

Highly recyclable pH-responsive lignin-polyethylene glycol (L-PEG) was synthesized to achieve enhanced lignocellulosic hydrolysis and recycling cellulase. The performance of L-PEG could be easily regulated by adjusting the molecular weight and the amount of PEG. The large molecular weight facilitated L-PEG to reduce the invalid adsorption of cellulase on lignin during hydrolysis and enhance its flocculation effect at around pH 3.0. L-PEG1000-40 obtained by adding 40 wt% (based on lignin) PEG1000 could effectively enhance the enzymatic hydrolysis of lignocelluloses and recover most of cellulase after hydrolysis through simply adjusting the pH of hydrolysate. During eucalyptus hydrolysis, using L-PEG1000-40 to recycle cellulase could not only save 40% cellulase, but also increase the glucose yield by 121%. Due to the low synthesis cost of L-PEG and the simple and convenient recovery operation, this new method is beneficial to the improvement of lignocellulosic saccharification process and the high-value utilization of lignin.Graphic abstract

The effects of lignosulfonate (LS) on enzymatic saccharification of pure cellulose were studied. Four fractions of LS with different molecular weight (MW) prepared by ultrafiltration of a commercial LS were applied at different loadings to enzymatic hydrolysis of Whatman paper under different pH. Using LS fractions with low MW and high degree of sulfonation can enhance enzymatic cellulose saccharification despite LS can bind to cellulase nonproductively. The enhancing effect varies with LS properties, its loading, and hydrolysis pH. Inhibitive effect on cellulose saccharification was also observed using LS with large MW and low degree of sulfonation. The concept of “LS-cellulase aggregate stabilized and enhanced cellulase binding” was proposed to explain the observed enhancement of cellulose saccharification. The concept was demonstrated by the linear correlation between the measured amount of bound cellulase and saccharification efficiency with and without LS of different MW in a range of pH.

Organic pollutants pose a serious threat to water environment, thus it is essential to develop high-performance adsorbent to remove them from wastewater. Herein, nitrogen-doped magnetic porous carbon (M-PLAC) with three-dimensional porous structure was synthesized from lignin to adsorb methylene blue (MB) and tetracycline (TC) in wastewater. The calculated equilibrium adsorption amount by M-PLAC for MB and TC was 645.52 and 1306.00 mg/g, respectively. The adsorption of MB and TC on M-PLAC conformed to the pseudo-second-order kinetic model. The removal of MB by M-PLAC showed fast and efficient characteristics and exhibited high selectivity for TC in a binary system. In addition, M-PLAC was suitable for a variety of complex water environments and had good regeneration performance, demonstrating potential advantages in practical wastewater treatment. The organic pollutant adsorption by M-PLAC was attributed to electrostatic interaction, hole filling effect, hydrogen bonding, and the π-π interaction.

Pickering emulsion stabilized by lignin particles has many advantages such as high flexibility, natural non-toxicity, anti-oxidation, and anti-ultraviolet. In order to promote the application of industrial lignin in the field of Pickering emulsions, this study has done comparatively systematic and basic research on Pickering emulsions stabilized by lignin particles. The emulsification effects of lignin particles on cyclohexane and n-decanol which have opposite polarity were compared firstly under different oil-water ratios. It was found that stable emulsions formed when the three-phase contact angle of oil/water/lignin was closer to 90°. The weakly polar cyclohexane could be well-emulsified by lignin particles, while the strong polar n-decanol could not. Cyclohexane was used as the oil phase to discuss the emulsification ability of lignin particles under different concentrations or with different particle sizes. The results show increasing the concentration of lignin particles or reducing the particle size can improve the emulsification performance.

Nonionic surfactants could effectively improve the enzymatic hydrolysis efficiency of lignocellulose, while small molecule anionic and cationic surfactants usually inhibited the enzymatic hydrolysis. The results showed that the anionic surfactant sodium dodecyl sulfate (SDS) could improve the enzymatic hydrolysis efficiency of Avicel at the concentration range of 0.1–1 mM, but it did inhibit enzymatic hydrolysis at higher concentration. Cationic surfactant cetyltrimethylammonium bromide (CTAB) was used to regulate the surface charge of SDS; thereby catanionic surfactant SDS-CTAB was formed. The effect of SDS-CTAB catanionic surfactant with varied molar ratios on the enzymatic hydrolysis of pure cellulose and corn stover at various enzymatic hydrolysis environments was investigated. SDS-CTAB could increase the enzymatic hydrolysis of corn stover at high solid loading from 33.3 to 42.4%. Using SDS-CTAB could reduce about 58% of the cellulase dosage to achieve 80% of the enzymatic hydrolysis of corn stover. SDS-CTAB catanionic surfactant could regulate the surface charge of cellulase in the hydrolyzate and reduce the non-productive adsorption of cellulase on the lignin, thereby improving the enzymatic hydrolysis efficiency of lignocellulose.

This study revealed that cellulose enzymatic saccharification response curves of lignocellulosic substrates were very different from those of pure cellulosic substrates in terms of optimal pH and pH operating window. The maximal enzymatic cellulose saccharification of lignocellulosic substrates occurs at substrate suspension pH 5 . 2 – 6 . 2 , not between pH 4 . 8 and 5 . 0 as exclusively used in literature using T. reesi cellulase. Two commercial cellulase enzyme cocktails, Celluclast 1.5L and CTec2 both from Novozymes, were evaluated over a wide range of pH. The optimal ranges of measured suspension pH of 5.2–5.7 for Celluclast 1.5L and 5.5–6.2 for CTec2 were obtained using six lignocellulosic substrates produced by dilute acid, alkaline, and two sulfite pretreatments to overcome recalcitrance of lignocelluloses (SPORL) pretreatments using both a softwood and a hardwood. Furthermore, cellulose saccharification efficiency of a SPORL-pretreated lodgepole pine substrate showed a very steep increase between pH 4.7 and 5.2. Saccharification efficiency can be increased by 80 % at cellulase loading of 11.3 FPU/g glucan, i.e., from approximately 43 to 78 % simply by increasing the substrate suspension pH from 4.7 to 5.2 (buffer solution pH from 4.8 to 5.5) using Celluclast 1.5L, or by 70 % from approximately 51 to 87 % when substrate suspension pH is increased from 4.9 to 6.2 (buffer solution pH from 5.0 to 6.5) using CTec2. The enzymatic cellulose saccharification response to pH is correlated to the degree of substrate lignin sulfonation. The difference in pH-induced lignin surface charge, and therefore surface hydrophilicity and lignin–cellulase electrostatic interactions, among different substrates with different lignin content and structure is responsible for the reported different enhancements in lignocellulose saccharification at elevated pH.