INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2021
·Vol. 23
·期 1
·413
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IF 5.924
Wen-Jie Guo,Jia-Kun Xu,Sheng-Tao Wu,Shu-Qin Gao,Ge-Bo Wen,Xiangshi Tan,Ying-Wu Lin
The treatment of environmental pollutants such as synthetic dyes and lignin has received much attention, especially for biotechnological treatments using both native and artificial metalloenzymes. In this study, we designed and engineered an efficient peroxidase using the O2carrier myoglobin (Mb) as a protein scaffold by four mutations (F43Y/T67R/P88W/F138W), which combines the key structural features of natural peroxidases such as the presence of a conserved His-Arg pair and Tyr/Trp residues close to the heme active center. Kinetic studies revealed that the quadruple mutant exhibits considerably enhanced peroxidase activity, with the catalytic efficiency (kcat/Km) comparable to that of the most efficient natural enzyme, horseradish peroxidase (HRP). Moreover, the designed enzyme can effectively decolorize a variety of synthetic organic dyes and catalyze the bioconversion of lignin, such as Kraft lignin and a model compound, guaiacylglycerol-β-guaiacyl ether (GGE). As analyzed by HPLC and ESI-MS, we identified several bioconversion products of GGE, as produced via bond cleavage followed by dimerization or trimerization, which illustrates the mechanism for lignin bioconversion. This study indicates that the designed enzyme could be exploited for the decolorization of textile wastewater contaminated with various dyes, as well as for the bioconversion of lignin to produce more value-added products.Keywords:heme enzymes;protein design;dye-decolorizing peroxidase;kraft lignin bioconversion
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RSC Advances
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2021
·Vol. 11
·期 56
·35280-35286
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IF 3.361
Jingliang Xu,Xinhang Hu,Md Asraful Alam,Gul Muhammad,Yongkun Lv,Minghai Wang,Chenjie Zhu,Wenlong Xiong
Zn/MnO2 batteries, one of the most widely studied rechargeable aqueous zinc-ion batteries, suffer from poor cyclability because the structure of MnO2 is labile with cycling. Herein, the structural stability of α-MnO2 is enhanced by simultaneous Al3+ doping and lignin coating during the formation of α-MnO2 crystals in a hydrothermal process. Al3+ enters the [MnO6] octahedron accompanied by producing oxygen vacancies, and lignin further stabilizes the doped Al3+ via strong interaction in the prepared material, Al-doped α-MnO2 coated by lignin (L + Al@α-MnO2). Meanwhile, the conductivity of L + Al@α-MnO2 improves due to Al3+ doping, and the surface area of L + Al@α-MnO2 increases because of the production of nanorod structures after Al3+ doping and lignin coating. Compared with the reference α-MnO2 cathode, the L + Al@α-MnO2 cathode achieves superior performance with durably high reversible capacity (∼180 mA h g−1 at 1.5 A g−1) and good cycle stability. In addition, ex situ X-ray diffraction characterization of the cathode at different voltages in the first cycle is employed to study the related mechanism on improving battery performance. This study may provide ideas of designing advanced cathode materials for other aqueous metal-ion batteries.
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INDUSTRIAL CROPS AND PRODUCTS
·
2021
·
IF 5.645
Ming Li,Yunxiu Jia,Xin Shen,Tao Shen,Zhuotao Tan,Wei Zhuang,Gulin Zhao,Chenjie Zhu,Hanjie Ying
This study prepared ternary composites PBAT/thermoplastic starch (TPS)/lignin containing 20, 30 and 40 wt% of TPS/lignin fillers via thermal compounding, and found that lignin imposes compatibilization effect on PBAT and TPS. Thermal analysis shows that the incorporation of lignin results in higher thermal stability, reduced crystallization temperatures, broader crystallization exotherms and increased T g due to the rigid aromatic structure of lignin. Tensile tests exhibit that strain at break and tensile strength reaches a maximum at loading 10 wt% of lignin. The reinforcement of lignin is reflected as the enhanced elastic modulus, Shore-D hardness, and more prominent yielding behavior of the composites. Rheological and microscope measurements show that the incorporation of lignin leads to higher approximation to theoretical Han curve, and reduced TPS particle size in the composites, indicating that lignin improves the interfacial compatibility between the PBAT and TPS phases. Contact angle and water absorption results demonstrate that lignin improves the hydrophobicity and water repelling ability of the composites, which are favorable for products with prolonged mechanical properties and shelf life.
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Journal of Cleaner Production
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2021
·
IF 9.297
Huiting Lin,Shijie Qiu,Zhihao Wu,Xiaoxia Ye,Minghua Liu
Efficient removal of oxytetracycline hydrochloride (OTC) from wastewater is of great significance but extremely challenging. Herein, a novel adsorbent lignin-based multi-metal ferrite biochar (FeNiZn-LBC) was synthesized through pyrolysis with controllable temperature and hydrothermal reaction using lignin of sinocalamus oldhami as raw material. The adsorption property of FeNiZn-LBC for OTC was systematically researched, and the results displayed that adsorption of FeNiZn-LBC to OTC accorded with the Langmuir model and the equilibrium adsorption capacity was 476 mg g −1 . Notably, FeNiZn-LBC can be regenerated with 0.100 mol L −1 NaOH. Additionally, we raised rational explanations for the mechanisms of adsorption behavior based on the zeta potential and XPS spectra. The adsorption of FeNiZn-LBC for OTC was mainly controlled by the electrostatic interactions, hydrogen bonds and complexation involving FeNiZn-LBC and OTC, especially the metal-oxide bond (M-O) generated after loaded with multi-metal ferrite played a positive role in the removal of OTC from water. Our work highlighted the potential of FeNiZn-LBC for excellent adsorption of OTC in next generation.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
·
IF 6.953
Guifeng Liu,Can Jin,Shuping Huo,Zhenwu Kong,Fuxiang Chu
A series of lignin-based epoxy resins (LEPs) were prepared by the reaction of epichlorohydrin with lignin oligomers derived from partial reductive depolymerization of lignin. To overcome the high viscosity and brittleness defects in practical applications, the LEPs were blended with renewable epoxied cardanol glycidyl ether (ECGE) and then cured with methyltetrahydrophthalic anhydride (MeTHPA) to form high-performance epoxy thermosets. The effects of degree of lignin depolymerization , chemical composition of lignin oligomers and dosage of ECGE on thermal and mechanical properties of the cured products were investigated. The LEP/MeTHPA thermosets exhibited good thermal and mechanical properties. Especially, by separating monomer-rich fractions from lignin oligomers, the thermal and mechanical properties of the cured product were improved obviously. Notably, the incorporation of ECGE also possessed a positive effect on reinforcing and toughening the cured products. With 20 wt% ECGE loadings, the tensile, flexural and impact strength of the cured product reached the maximum value of 77 MPa, 115 MPa and 14 kJ/m 2 , respectively, which were equivalent to the commercial bisphenol A epoxy resins thermosets. These findings indicated that the novel bio-based epoxy resins from lignin oligomers and cardanol could be utilized as renewable alternatives for BPA epoxy resins.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Xiangchen Kong,Chao Liu,Yuyang Fan,Weicong Xu,Rui Xiao
Production of jet fuel precursors from waste kraft lignin through a depolymerization and hydrodeoxygenation (DHDO) method with a complex copper acid catalyst is reported. The kraft lignin undergoes a high degree of depolymerization, deoxygenation, hydrogenation, and C–C coupling. Monomers and dimers with molecular weights in the ranges of <200 Da and 354–452 Da are obtained with optimized yields reaching 93.29 and 39.30 C% at 360 °C for 8 h, while trimers and oligomers with higher molecular weights are also generated with lower contents. The high carbon yields of monomers and dimers are given by the incorporation of methanol solvent. The double bond equivalent (DBE) and polydispersity index (PDI) decrease from 14.77 and 2.77 in kraft lignin to 9.05 and 1.35 in the products, while the high heating value (HHV) increases from 24.53 to 36.47 MJ/kg after reaction. Furthermore, over 45% of the optimized products have boiling points in the range of that of commercial jet fuel (60–280 °C). All these results demonstrate the appropriate properties of the products from kraft lignin DHDO as potential jet fuel precursors.
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Frontiers in Energy Research
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2021
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IF 4.008
Li Jiayi,Zhou Wei,Huang Yuming,Gao Jihui
Replacing the oxygen evolution reaction (OER), which is of high energy consumption and slow kinetics, with the more thermodynamically favorable reaction at the anode can reduce the electricity consumption for hydrogen production. Here we developed a lignin-assisted water electrolysis (LAWE) process by using Ti/PbO2 with high OER overpotential as the anode aimed at decreasing the energy consumption for hydrogen production. The influence of key operating parameters such as temperature and lignin concentration on hydrogen production was analyzed. Compared with alkaline water electrolysis (AWE), the anode potential can be decreased from 0.773 to 0.303 (V vs. Hg/HgO) at 10 mA/cm2 in LAWE, and the corresponding cell voltage can be reduced by 546 mV. With increasing the temperature and lignin concentration, current density and H2 production rate were efficiently promoted. Furthermore, the anode deactivation was investigated by analyzing the linear sweep voltammetry (LSV) and cyclic voltammetry (CV) tests. Results showed that the anode deactivation was affected by the temperature.
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INDUSTRIAL CROPS AND PRODUCTS
·
2021
·
IF 5.645
Liping Tan,Yongchao Zhang,Weihua Zhang,Rongwen Zhao,Yue Ru,Tongjun Liu
Valorization of lignin is imperative since lignin is still an underutilized biomaterial. Herein, a facile fabrication method for lignin-based magnetic biosorbent (LMB) is proposed via assembling magnetic inorganic particles (Fe 3 O 4 ) on lignin in-situ for eliminating heavy metal ions (HMIs) from wastewater without the utilization of organic solvents. Chemical and structural characterizations, which were determined by different analytical tools, including Fourier transform infrared (FTIR), Scanning electron microscope (SEM), X-ray diffraction (XRD), High-resolution transmission electron microscopy (HRTEM), and X-ray photoelectron spectroscopy (XPS) confirmed that LMB was successfully formed via the feasible and green process. Then, LMB was found to exhibit highly effective removal performance for HMIs. The adsorption capacity of the LMB reached 152.58 mg/g for Pb 2+ and 46.81 mg/g for Cu 2+ , with equilibrium attained within 30 min. Adsorption kinetics and isothermal adsorption of lead and copper ions by LMB were also examined. This study delivers a new perspective on lignin valorization for lignocellulose biorefineries and establishes a path for synthesizing a cost-efficient and green adsorbent for removing HMIs from wastewater.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2021
·
IF 4.952
Qinglan Wu,Mingfei Ren,Xinxia Zhang,Cheng Li,Ting Li,Zhi Yang,Zhengxing Chen,Li Wang
Rice bran, an underutilized by-product obtained from outer rice layers, has received wide interest due to its abundance, eco-friendliness, and low cost. In this research, cellulose , hemicellulose and lignin as the main components of rice bran were fractionated, and their Cd(II) adsorption capacity, behavior and mechanism were further studied. The adsorption capacity of cellulose for Cd(II) was 5.79 mg/g within the equilibrium time of 10 min, which was 1.8 and 3.6 times those of hemicellulose and lignin, respectively. The Cd(II) adsorption onto cellulose exhibited monolayer surface behavior, whilst the heterogeneous adsorption behavior was observed for hemicellulose and lignin. These differences were related to the discrepancy of morphology and chemical composition in three polymers. The multi-hole sticks morphology of cellulose and porous blocky structure of hemicellulose were observed, while lignin showed compact and agglomerated blocky structure. Cellulose had numerous available adsorption sites including the oxygen-containing functional groups, which bonded with Cd(II) driven by chemical interaction. In conclusion, it highlights that cellulose from rice bran has the great potential of being applied as adsorbent for the Cd(II) removal.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Xiaoqi Wang,Mo Qiu,Yiwei Tang,Jirui Yang,Feng Shen,Xinhua Qi,Yingliang Yu
Sulfonated lignin-derived ordered mesoporous carbon (OMC-SO 3 H) solid acid was synthesized through solvent evaporation induced self-assembly (EISA) method followed by sulfonation , using lignin as carbon precursor and glyoxal as cross-linking agent during the preparation process. The as-synthesized OMC-SO 3 H exhibited a typical 2D hexagonal meso-structure (space group p6mm ) and showed a good catalytic performance for the catalytic conversion of hemicellulose-derived xylose to furfural. A highest furfural yield of 76.7% with 100% xylose conversion was achieved at 200 °C for 45 min in γ-valerolactone (GVL)-water (85:15 v /v%) mixture. The lignin-derived OMC-SO 3 H solid acid catalyst showed superior stability and reusability, and was also applicable to the catalytic production of furfural from xylan . This work provides a promising strategy for the synthesis of ordered mesoporous carbon solid acid from green and sustainable lignin biomass resource, which has wide range of applications in the utilization of cellulose and hemicellulose .
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2021
·
IF 5.645
Hao-Nan Zhang,Hao Ren,Hua-Min Zhai
The structure of kraft lignin is heterogeneous and the reaction activity is low due to the complicated and somewhat uncertain chemical reactions under the strong alkali and high temperature conditions of kraft pulping chemistry. At present, people still lack understanding of its structure, so it is difficult to be used as high quality industrial raw material for many years despite its huge output. In this paper, the phenolation potential of industrial Spruce Kraft Lignin (SKL) in phase separation system was explored. Compared with previous studies on phase separation reaction, due to the direct use of lignin as feedstock , sulfuric acid would only act as a phenolation catalyst, and is no longer used for swelling cell walls and hydrolyzing carbohydrates , so a modest reduction of acid concentration is feasible. In the phase separation system, the benzyl position of lignin was activated to selectively graft the p -cresol groups. Due to the protection of organic phase on lignin, the breakage of the β linkages and the condensation reaction of lignin were effectively prevented, so the original structure of lignin was well preserved. In order to capture the detailed structural changes of lignin after phenolation in phase separation system, FT-IR, GPC and quantitative NMR techniques ( 1 H-NMR, 31 P-NMR and 2D-NMR) were used to analyze the changes of main functional groups, linkages and substructures of industrial lignin samples before and after phenolation. The results showed that the industrial spruce kraft lignin still have many active sites which can be modified by phenolation. And through p -cresol treatment, a kind of high activity industrial lignin with more phenolic hydroxyl groups, more uniform molecular size and higher purity was obtained. Then the molecular structure models of spruce kraft lignin before and after phenolation is proposed respectively based on the molecular weights, quantitative analysis of functional groups, linkages, substructures and introduced p -cresols. This will be helpful to understand the structural changes of industrial spruce kraft lignin during phenolation in phase separation system, and provide guidance for the high value utilization of this high activity industrial lignin in the future.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Jinhao Huang,Weifeng Liu,Xueqing Qiu,Zhikai Tu,Jinxing Li,Hongming Lou
In this work, the coordination-based energy sacrificial bonds have been constructed in the interphase between lignin and polyolefin elastomer to prepare high performance lignin-based thermoplastic elastomers (TPEs). The strength and toughness of lignin-based TPEs can be adjusted by choosing different nitrogen heterocyclic compounds as reactive assistants and Fe 3+ or Zn 2+ as metal coordination centers. It was demonstrated that 3-Amino-1,2,4-triazole with three nitrogen atoms in the heterocyclic ring and one nitrogen branch chain could form the most efficient coordination bond system and generate the best mechanical performance. The system with ferric iron as coordination center exhibited better enhancement effect than divalent zinc. By adjusting the nitrogen-containing reactive additives or metal salts as coordination centers, the mechanical performance of the lignin-based TPE can be regulated, which provides a method for making green bio-composites with good strength and toughness, and also promotes the high value utilization of lignin in polymer materials.
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