Biomass Conversion and Biorefinery
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2021
·Vol. 13
·期 14
·12581-12590
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IF 4.987
Liu Ruixia,Ding Tingting,Deng Pingping,Yan Xiaofan,Xiong Fuquan,Chen Jienan,Wu Zhiping
In order to improve the reaction activity of lignin and increase its utilization rate. Lignin extracted from poplar wood powder by deep eutectic solvent was degraded with hydrogen peroxide (H 2 O 2 ) and sodium hydroxide (NaOH) to obtain degraded deep eutectic solvent lignin (DES-lignin). The structures of DES-lignin and degraded DES-lignin were characterized by gel permeation chromatography (GPC), elemental analysis (EA), Fourier transform infrared spectroscopy (FT-IR), two-dimensional nuclear magnetic resonance spectroscopy (2D-HSQC NMR), and thermogravimetric analysis (TGA). The results indicated that the phenolic hydroxyl group of degraded DES-lignin increased by 39.62% and M w and M n decreased by 49.12% and 47.83%, respectively. C content decreased by 1.13%. The relative strength and S/G increased by 25.76% and 13.5%, respectively. The polymerization degree, β-O-4 linkages, and β-β linkages were decreased by 10.82%, 4.8%, and 4.2%, respectively. The residual residue increased by 8.3% at 800 °C. It showed that degraded DES-lignin had the advantages of strong activity, more reaction sites, narrow molecular weight distribution, less condensation structure, and thermal stability, which was more conducive to the high-value utilization of lignin.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Lei Jiang,Jia Liu,Shu He,An Liu,Jie Zhang,Haijun Xu,Wei Shao
The development of wearable devices promotes the multi-functional applications of conductive materials. Herein, highly stretchable PADL organohydrogels which consist of lignosulfonate nanoparticles (nano-LGS) doped poly(acrylic acid-co-2-(methacryloyloxy)ethyl trimethyl ammonium chloride) in Glycerol/H 2 O were prepared by a facile strategy. The organohydrogels exhibited strong adhesiveness, high self-healing ability and conductivity. Benefiting from the use of Glycerol/H 2 O binary solvent system, the fabricated organohydrogels showed anti-freezing property at −40 °C. Notably, nano-LGS acted as the enhancement particles to improve the mechanical properties, antibacterial activity as well as conductivity of PADL organohydrogels. Furthermore, strain sensors constructed by the organohydrogels can monitor human movements with high sensitivity (gauge factor of 7.91). Besides, they can detect handwriting as well. Thus, this work could provide a promising strategy for the fabrication of the self-healing and conductive organohydrogels in the application of wearable electronic devices.
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BIORESOURCE TECHNOLOGY
·
2020
·
IF 7.539
Juanhua Kong,Lixia Li,Qiang Zeng,Zhenping Cai,Yingying Wang,Hongyan He,Sijie Liu,Xuehui Li
Lignin is considered as a promising substitute for fossil resources, but its efficient conversion remains a huge challenge due to the structural complexity and immiscibility with typical solvents. Herein, a series of surfactant-free microemulsion reactors comprised of n -octane, water and n -propanol were designed and their corresponding phase behaviors alongside their ability to intensify oxidative depolymerization of lignin were explored. Experimental results show that the phenolic monomer yield improves substantially (40–500 wt%) by comparison with processes performed in a single solvent. Detailed characterizations also suggest that the above intensification is rationalized by the solubilization effect of microemulsion system and directional aggregation of lignin at the microemulsion interface.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Xinyan Chen,Bin He,Mi Feng,Dingwei Zhao,Jian Sun
As a natural aromatic polymer , lignin has great potential but limited industrial application due to its complex chemical structure. Among strategies for lignin conversion, biodegradation has attracted promising interest recently in term of efficiency, selectivity and mild condition. In order to overcome the issues of poor stability and non-reusability of enzyme in the biodegradation of lignin, this work explored a protocol of immobilized laccase on magnetic nanoparticles (MNPs) with rough surfaces for enhanced lignin model compounds degradation. Scanning electron microscope with energy dispersive spectrometer (SEM-EDS), flourier transformation infrared spectroscopy (FTIR) and thermal gravimetric analysis (TGA) were utilized to characterize the immobilization of laccase. The results showed a maximum activity recovery of 64.7% towards laccase when it was incubated with MNPs and glutaraldehyde (GA) with concentrations of 6 mg·ml −1 and 7.5 mg·ml −1 for 5 h, respectively. The immobilized laccase showed improved thermal stability and pH tolerance compared with free laccase, and remained more than 80% of its initial activity after 20 days of storage at 4 °C. In addition, about 40% residual activity of the laccase remained after 8 times cycles. Gas chromatography–mass spectrometry (GC–MS) was utilized to characterize the products of lignin model compound degradation and activation, and the efficiency of immobilized laccase was calculated to be 1–5 times that of free laccase. It was proposed that the synergistic effect between MNPs and laccase displays an important role in the enhancement of stability and activity in lignin model compound biodegradation.
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Polymers
·
2020
·Vol. 12
·期 3
·632
·
IF 3.426
Jianbing Guo,Jian Wang,Yong He,Hui Sun,Xiaolang Chen,Qiang Zheng,Haibo Xie
Soybean oil is beneficial to improve the compatibility between polylactide (PLA) and succinylated lignin (SAL), which leads to the preparation of a host of biobased composites containing PLA, SAL, and epoxidized soybean oil (ESO). The introduction of SAL and ESO enables the relatively homogeneous morphology and slightly better miscibility obtained from triply PLA/SAL/ESO composites after dynamic vulcanization compared with unmodified PLA. The rigidity of the composites is found to decline gradually due to the addition of flexible molecular chains. According to the reaction between SAL and ESO, theTgof PLA/SAL/ESO composites is susceptible to the movement of flexible molecular chains. The rheological behaviors of PLA/SAL/ESO under different conditions, i.e., temperature and frequency, exhibit a competition between viscidity and elasticity. The thermal stability of the composites displays a slight decrease due to the degradation of SAL and then the deterioration of ESO. The elongation at break and notched impact strength of the composites with augmentation of ESO increase by 12% and 0.5 kJ/m2, respectively. The triply biobased PLA/SAL/ESO composite is thus deemed as a bio-renewable and environmentally friendly product that may find vast applications.Keywords:lignin;polylactide composite;epoxidized soybean oil;dynamic vulcanization
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JOURNAL OF MEMBRANE SCIENCE
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2021
·
IF 8.742
Kaifeng Gu,Kaizhen Wang,Yong Zhou,Congjie Gao
Lignin is a widely used biomass material and has great application potential in papermaking, textile, petrochemical industry, etc. However, the traditional separation and extraction method for the lignin system has some disadvantages in energy consumption and separation effect, which greatly limited the application of lignin. The rapid development of nanofiltration (NF) membranes provides new ideas for solving this problem. The PEI/TGIC membrane with great alkali resistance (pH 7–14) by cross-linking polyethyleneimine (PEI) and triglycidyl isocyanurate (TGIC) was developed in this work. The influencing factors of membrane surface characteristics were discussed and membrane preparation parameters were optimized. The optimized PEI/TGIC membrane (prepared with 0.02% TGIC and 0.8% PEI) had the characteristics of high permeability and selectivity under low pressure (2 bar). The PEI/TGIC membrane was stable to the removal of PEG 1500 in an alkaline environment (pH 7–14). For lignin lye, the PEI/TGIC membrane could intercept the lignin (rejection>95%) while allowing the sodium hydroxide to almost completely penetrate. Under the operating pressure of 2 bar, the lye permeation flux could be maintained at 22 L m −2 h −1 . This work provided new ideas for the application of nanofiltration membranes and the treatment of lignin lye.
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GREEN CHEMISTRY
·
2021
·Vol. 23
·期 16
·6065-6075
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IF 10.182
Kai Rong,Jiale Wei,Yuchen Wang,Jingwei Liu,Zhen-An Qiao,Youxing Fang,Shaojun Dong
We developed a novel electrospinning strategy, using choline chloride–lactic acid (ChCl–LA) deep eutectic solvent (DES) as an electrospinning solvent to produce lignin fiber aerogels (LFA). The novel strategy is sustainable and cost-effective because no toxic or flammable volatile organic solvents were used and the precursors and waste were designed to be recycled. The fabricated LFA has the appearance of a piece of cotton, and the specific mass was calculated and found to be as low as 3 mg cm−3 with a porosity of over 99.7%. After stabilization and carbonization at a high temperature, the LFA can transform into lignin-based carbon fiber aerogels (LCFA). The LCFA has a high specific surface area (580 m2 g−1) and conductivity, and can be used as an electrochemical electrode material. We made supercapacitor electrodes using the LCFA, the specific capacitance of which is 155 F g−1, much higher than that of commercial multi-wall carbon nanotubes (39 F g−1) at a current density of 0.5 A g−1. The LCFA also have a high electrochemical cycling stability. For the supercapacitor electrodes, only a 2% decrease was observed after 5000 cycles. Moreover, all waste in this work was recycled and reused five times to achieve electrospinning with almost no waste.
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FUEL
·
2021
·
IF 6.609
Mingxing Zhao,Jun Hu,Shiliang Wu,Liu Yang,Xue An,Peng Yuan,Ping Lu
Cyclohexanols, promising oxygenated fuel additives and value-added chemicals, can be obtained by hydrodeoxygenation (HDO) of lignin-derived phenolics. Here, an N-doped bimetallic RuCoN x /NC catalyst was facilely prepared for HDO by direct pyrolysis of chitin impregnated with precursors of Ru and Co. Characterization of RuCoN x /NC with N 2 sorption, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and NH 3 temperature-programmed desorption (NH 3 -TPD) reveal that the metallic particles of electron-deficient Ru species and electron-enriched Co species were uniformly anchored on the micro-mesoporous N-doped carbon matrix with high dispersion and nano-scale size. The abundant accessible active sites and continuous spillover of H from Ru to Co make RuCoN x /NC an excellent HDO catalyst. 4-Propylguaiacol, a typical phenolic compound from lignin degradation, was hydrodeoxygenated into 92% 4-propylcyclohexanol over RuCoN x /NC at 210 ℃. With temperature increasing, propylcyclohexane became the major product, possessing 95% selectivity at 280 °C after 6 h. Reusability tests show that RuCoN x /NC can be recycled four times without the loss of conversion and initial selectivity. HDO of other phenolic compounds confirms the general applicability of RuCoN x /NC.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2019
·
IF 4.784
Tao Zheng,Dingming Zhong,Dafeng Zheng,Fengli Bao,Jianmin Zheng,Xueqing Qiu
In order to develop a biomass-based superplasticizer, kraft lignin (KL) was grafted with isopentenol polyoxyethylene ether (TPEG) to prepare a novel macromonomer (KL-TPEG). It was shown that the retention ratio of the aliphatic C C bond increased from 81.07% to 90.20% with the increase of m(TPEG)/m(KL). When the grafting ratio was increased, the average number of TPEG grafted on one KL molecule was approximately 1.4, 3.1, 4.6, 6.2 and 7.6. The star-like structure was also confirmed by FT-IR, 1 H NMR and GPC. KL-TPEG had favorable surface activity and dispersion stability on the cement particles. It was illustrated that the shear stress and shear viscosity of the cement slurries with KL-TPEG were significantly less than that of blank slurry. The dispersion-retention ability of KL-TPEG on the slurry was also gradually enhanced with the increase of the grafting ratio of TPEG. It was seldom reported on the biomass-based TPEG. Through modified with KL, the rheology behavior and the dispersion-retention ability of TPEG was greatly improved, and the cost of TPEG was also reduced, thus this study not only promoted the development of biomass-based macromonomer, but also helped for the high value utilization of lignin.
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Chemical Science
·
2019
·Vol. 10
·期 45
·10640-10646
·
IF 9.556
Jingjing Zhang,Qingli Qian,Ying Wang,Bernard Baffour Asare Bediako,Jiang Yan,Buxing Han
Currently, ethanol is produced via hydration of ethene or fermentation of foods. Lignin and CO2 are abundant, cheap and renewable feedstocks. Synthesis of ethanol using the lignin or its derivatives is of great importance, but is a great challenge and has rarely been reported. Herein, we propose a route to synthesize ethanol from CO2, H2, and lignin or various aryl methyl ethers, which can be derived from lignin. The reaction could be effectively conducted using Ru–Co bimetallic catalyst and the TON of ethanol could reach 145. Interestingly, ethanol was the only liquid product when lignin was used. A series of control experiments indicate that ethanol was formed via cleavage of aryl ether bond, reverse water gas shift (RWGS) reaction, and C–C bond formation. This protocol opens a way to produce ethanol using abundant renewable resources.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
YinChen Chen,Shiyu Fu,Hui Zhang
Acetic acid lignin (AAL) obtained from Bagasse was used as a partial substitute of polyols for polyurethane (PU) adhesive due to the presence of reactive sites, i.e. aliphatic and aromatic hydroxyl groups, in its structure. To improve its reactivity, lignin is partly demethylated before the copolymerization with polyisocyanate. The demethylation , catalyzed by hydrobromic acid solution under heating conditions, resulted in a decrease of methoxy groups on the phenyl ring and the increase of phenolic hydroxyl groups . It is found that 120 ℃ is the preferred temperature for the demethylation resulted in a 36.5 % increase in hydroxyl content of lignin up to 5.25 mmol/g. Lignin-based polyurethane adhesives were prepared in two steps including preparing a prepolymer based on mixtures of toluene-2,4-diisocyanate (TDI) and unmodified or demethylated lignin, and then the polymerization was completed by adding polyethylene glycol (PEG). The mass ratio (1:1) of TDI: (lignin + PEG) in the compositions was here investigated. The results indicated that the presence of lignin (with and without demethylation) in polyurethane adhesives increased the glass transition temperature , Young’s modulus, and elongation at break. Particularly, the tensile strength was increased by 15–36 MPa with the addition of 10–30 wt% of lignin. Lignin with higher amount of hydroxyl groups prepared by partly demethylation is better integrated into the three-dimensional cross-linking networks of the covalent polymer as a substitute of polyols. Compared to those PU adhesives based on the raw AAL, the adhesives prepared by demethylated lignin have higher tensile strength and thermal stability. It indicates that the demethylation is effective and it is a good strategy to prepare lignin-based PU adhesive with favorable mechanical properties .
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MACROMOLECULES
·
2019
·
IF 5.997
Weifeng Liu,Chang Fang,Shengyu Wang,Jinhao Huang,Xueqing Qiu
High-performance lignin-containing polyurethane elastomers (LPUes) were successfully synthesized via partially substituting petroleum-derived polyols with depolymerized enzymatic hydrolysis lignin (DEL). The influences of DEL on the structure, thermostability, mechanical performance, and thermal reprocessability of LPUes were systematically studied. The tensile strength and toughness of PUes were significantly enhanced after the introduction of DEL, with the maximum tensile strength reaching up to 60.7 MPa and the toughness up to 263.6 MJ/m3. The enhancement for the strength and toughness was attributed to the dual cross-linking network structure and the interfacial hydrogen bonds between lignin and the PU matrix, which were demonstrated to facilitate the orientation of chain segments and lead to strain-induced crystallization and self-reinforcement. LPUes also exhibited much better elasticity than the control sample without lignin and could maintain excellent mechanical performance after being hot reprocessed.
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