Sustainable Chemistry and Pharmacy
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2021
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IF 4.508
Liuqun Gu,Meifeng Wang,Hui Li,Kai Ni Teh,Yiqun Li,Ye Liu
A new type of modified lignin, lignin-p-Boc, was obtained through reaction with di- tert -butyl dicarbonate (Boc 2 O) in aqueous media catalyzed by 4-dimethylaminopyridine (DMAP). Boc modification occurred regardless of type of lignin, was tunable, and proceeded well in recovering lignin at high purity from sodium lignosulfonate (a common byproduct from pulping industry; lignin content: 60%). Lignin-p-BOC was demonstrated as a potential reactive filler in green plastic and as a potential crosslinker in design of bioresorbable composite polymeric implants. Furthermore, the effect of the modification on breakdown rate of alkali lignin by microbes was investigated, and results showed that the modification substantially decreases the breakdown rate. The tunable Boc modification process was designed via a system thinking, including availability of raw lignin, economical/green modification, potentiality of drop-in-change to current thermoplastic processing, modification impact on microbial degradability/disposed environment at the end of use life; hence the holistic consideration makes this alternative method for upgrade of technical lignins very practical for future industrial application. Via “ in-situ ” forming “easily breakable covalent bonds” with existing thermopolymers inside, Lignin-p-BOCs are also promising to play an important role as both excellent binders via “random match” and reductants in transforming linear plastic waste into circular plastics.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2020
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IF 3.905
Qingguo Zhou,Zhongyang Luo,Guoxiang Li,Simin Li
Lignin pyrolysis is a promising method for the sustainable production of phenolic compounds from biomass. However, detailed knowledge about the radicals involved in this process and their influence during the coking is missing. Herein, we report on the pyrolysis of guaiacol, a lignin monomer at 600 °C under inert and hydrogen gas conditions. During the pyrolysis process, the formed radicals were detected by two improved electron paramagnetic resonance spectroscopy methods. Successfully observed o-phenyl semiquinone radical anion, cyclopentadienyl radical, methyl radical, hydroxyl radical, methoxy radical, phenyl radical, phenoxy radical, etc. during the pyrolysis of guaiacol, as well as the changes of related radicals in different pyrolysis stages. It was found that o-semiquinone radical anions and cyclopentadienyl radicals were the key free radicals in the generation of coke and tar during the pyrolysis process. And through hydrogenation pyrolysis experiments, it was verified that the relative content of o-semiquinone radical and the solid coke were reduced with a hydrogen supply source. Our results showed that by controlling the key free radicals in the coking process, the formation of coke can be suppressed and the conversion efficiency can be improved.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Wenliang Wang,Zhenhao Ma,Xingjin Zhao,Shiwei Liu,Liping Cai,Sheldon Q. Shi,Yonghao Ni
Microwave absorbents play a vital role in governing the monomeric products from lignin during the microwave-assisted depolymerization (MAD) process. The influence of various microwave absorbents on the conversion efficiency and lignin monomeric products in a dynamic vapor flow reaction system was investigated. Results showed that the selected microwave absorbents could linearly and rapidly heat lignin from 200 to 500 °C within 8 min under a microwave power of 1000 W. The yields of liquid products, guaiacols, and phenols were increased linearly with the heating rate (°C/min). The high microwave absorptivity of absorbents promoted the formation of liquid products and phenolic compounds. To offer further support, the use of MoS2 with a very high microwave absorptivity (185.0 °C/min) showed very high yields of liquid products (34.1 wt %) and phenolics (32.1 wt %). This work provided an effective methodology to enhance the lignin conversion efficiency to monomeric products using microwave absorbents.
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ACS Sustainable Chemistry & Engineering
·
2020
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IF 7.632
Chongbo Cheng,Pengfei Li,Wenbing Yu,Dekui Shen,Xiaoxiang Jiang,Sai Gu
Lignin containing numerous phenylpropane units is considered to be a renewable and abundant resource for the production of value-added aromatic chemicals. A series of nonprecious metal/bimetallic catalysts were prepared for the catalytic hydrogenolysis of organosolv poplar lignin (OPL) in ethanol/isopropanol solvent in this work. Effects of Ni/C, Cu/C, NiCu/C, and NiW/C catalysts on OPL depolymerization were investigated, where the NiCu/C catalyst was found to be optimal for the conversion of OPL to phenolic monomers at a yield of 63.4 wt % at 270 °C for 4 h without external H2. The synergistic effect of mixed solvent was remarkable during the catalytic hydrogenolysis process, leading to the increased yield of monomer products. The catalytic process of OPL conversion and possible reaction route of ethanol/isopropanol solvent were proposed with regard to the analysis of products and fresh/spent catalysts. The effects of reaction temperature, reaction time, catalyst recyclability, solvent recyclability, and feedstock adaptability were investigated in view of bio-oil and monomer yields. This work provides an economical and sustainable method for the efficient conversion of lignin to high-value chemicals.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Zhengyi Zhang,Jiaoman Li,Yan Zhang,Zhenfu Jin
Lignin, which is crosslinked by ether and carbon‑carbon linkages, is a highly branched polymer consisting of phenyl propane units. And owing to the abundant phenolic hydroxyl groups and its structural heterogeneous characteristics, lignosulfonate, considered as a renewable aromatic macropolymer, can be used as co-curing agent in EP thermoset systems. In this study, kinetics of lignosulfonate (LS) and partially depolymerized lignosulfonate (DLS) as co-curing agents for applications to EP thermoset were discussed with the differential scanning calorimetry (DSC) measurement. The activation energy ( E a ) and dynamic modeling of curing reaction were obtained by the methods of non-isothermal kinetic analysis reported by Kissinger and Ozawa. The glass transition temperature ( T g ) was determined by DSC and mechanical properties of epoxy resins were carried out using the Universal Testing Machine. The LS dropped the exothermic peak temperature and E a of curing reaction of EP thermoset. Those of DLS were more active than the higher molecular weight lignosulfonate. The EP thermoset cured with DLS (EP-DLS) exhibited much higher reactivity, and the curing reaction could be occurred at lower temperature. The T g of EP-DLS has risen by 10 °C compared with the case without lignosulfonate. The tensile strength , elongation at break and impact strength of EP-DLS rose by 28.7%, 52.5% and 53.5%, respectively, than those of the epoxy resin cured with LS (EP-LS).Molecular weight of lignosulfonate could be an important factor of the curing reaction of EP thermoset. The high performance EP thermoset could be obtained by partially depolymerized lignin as co-curing agents.
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PubMed
高影响因子
ELECTROCHIMICA ACTA
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2020
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IF 6.215
Meilian Cao,Wanli Cheng,Xiaohui Ni,Yi Hu,Guangping Han
The lignin-based multi-channels carbon nanofibers (MCNFs) @ SnO 2 nanocomposites with various microstructures are synthesized via co-electrospinning by regarding Poly (vinyl pyrrolidone) (PVP)–SnCl 2 ·2H 2 O as shell materials and lignin-Poly (methyl methacrylate) (PMMA) at different mass ratios as core materials, followed by heat treatment and acid treatment. The experimental results show that when the mass ration of lignin to PMMA in the core region is 5:5, the obtained nanocomposites possess hierarchical internal channels, porous surface, and high specific surface area. This optimized nanocomposite as supercapacitor electrode shows high specific capacitance of 406 F g −1 at current density of 0.5 A g −1 . In addition, the electrode exhibits unexceptionable cycling stability with only 5% capacitance decay over 10 000 cycles at 10 A g −1 . Furthermore, the symmetric supercapacitor using the optimized nanocomposites as electrodes possesses remarkable power and energy densities. The superior electrochemical performance of nanocomposites is benefited from the hierarchical structures of MCNFs, faradaic pseudocapacitance of SnO 2 , and pore-forming effect of SnCl 2 ·2H 2 O. The unique hierarchical nanocomposites show great potential in future development of lignin-based low-cost, non-toxic and eco-friendly carbon materials for high-performance energy storage devices.
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MATERIALS LETTERS
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2020
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IF 3.204
Yan Zhao,Minyue Wen,Chunhu He,Changlang Liu,Zongru Li,Yin Liu
The lignin residue produced by straw fermentation or straw acid hydrolysis is used as a carbon source to synthesize graphene. After adding tetrahydrofuran as a modifier and Fe(NO 3 ) 3 as a catalyst to lignin for pretreatment, the resulting product was heat treated at 900℃ for 3 h. The prepared graphene was characterized by XRD, Raman, HRTEM, and the electrochemical properties of the prepared graphene also were tested. The results of this study open up a new way for the efficient preparation of graphene based on renewable resources lignin. The prepared lignin-based graphene was used for electrochemical testing and found to be a good electrode material for super capacitors.
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RENEWABLE ENERGY
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2019
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IF 5.439
Qing-Lu Song,Yun-Peng Zhao,Fa-Peng Wu,Guo-Sheng Li,Xing Fan,Rui-Yu Wang,Jing-Pei Cao,Xian-Yong Wei
Low aromaticity and a large number of oxygen-bridged bonds among the aromatic structural units of lignin make it possible to obtain chemicals directly. A novel Co/ [email protected] catalyst with high activity towards hydrogenolysis of lignin-derived aryl ethers was synthesized according to the pyrolysis process of a predesigned ZIF-67. According to the results of characterization by powder X-ray diffraction (XRD), N 2 adsorption-desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS), Co was reduced by the carbonized organic linker of ZIF-67, and N was doped into the carbon skeleton of the catalyst. The effects of holding time, temperature, and initial H 2 pressure on the catalytic performance of Co/ [email protected] were evaluated in the selective hydrogenolysis of benzyl phenyl ether (BPE). BPE was completely converted and the selectivity of monomer reached to 98.2% under optimized reaction conditions. The C alk -O bond in BPE was first dissociated to form toluene and phenol, and then phenol was rapidly hydrogenated to form cyclohexanol. Furthermore, the Co/ [email protected] catalyst shows high activity for hydroprocessing and selective cleavage of other lignin-derived aryl ethers, including phenylethyl phenyl, diphenyl ether, dibenzyl ether, dinaphthalene ether, guaiacol, anisole and veratrole.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Haixu Wang,Weifeng Liu,Zhikai Tu,Jinhao Huang,Xueqing Qiu
In this work, half the mass of carbon black (CB) was replaced by lignin for preparation of high-performance nitrile rubber/poly(vinyl chloride) composites via constructing interfacial Zn2+-based coordination bonds. It was demonstrated that lignin played a significant role as a natural ligand to form the Zn2+-based coordination interactions in the interphase between lignin and a rubber matrix. The tensile strength and Young’s modulus of the composites were significantly enhanced by the Zn2+-based coordination bonds owing to the dynamic fracture of coordination bonds. The thermo-oxidative aging resistance of the composites was improved by lignin and could be conveniently regulated by the content of ZnCl2 and sulfur. The high-temperature oil resistance of the composites also benefited from the partial substitution of CB by lignin and incorporation of the metal coordination bonds. This work opens a facile method for the potential application of green lignin in rubber–plastic composites through a conventional rubber compounding process.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Liangliang Zhu,Ben Dang,Kairui Zhang,Jun Zhang,Mei Zheng,Ning Zhang,Guanben Du,Zhijun Chen,Rongbo Zheng
Bioplastics (BPs) prepared from lignocellulose are an excellent replacement for petrochemical-plastics (PCPs) due to their renewability and biodegradability. The presence of residual/added/regenerated lignin reduced the water sensitivity; however, these BPs possessed a deep color and low transmittance and were prone to photodegradation. Herein, we developed a UV- and water-insensitive, colorless, transparent, and sustainable wood-derived BP (W-BP) by pressing delignified wood (DW) with 0.21% lignin and abundant hydrophobic crystal plane (200) of cellulose. The DW was obtained by the pretreatment of the wood sample with NaOH/Na2SO3 followed by H2O2 steam conditioning. The abundant hydrophobic crystal plane (200) of cellulose in DW was demonstrated by a large ratio of the crystal plane (200) to (110), the presence of two-dimensional (2D) nanosheets of defibrated cellulose, and a low moisture uptake of 8.7% of the freeze-dried DW. The aged W-BP with a thickness of about 50 μm displayed good photostability with a ΔE* value of 2.3 and a transparency of 84% transmittance at 550 nm. Additionally, W-BP also possessed water stability with a wet tensile strength of 74 MPa and a low water uptake of 28.3%. These values exceeded those of lignocellulosic BPs and some commercial PCPs. The W-BP could replace transparent PCPs and provide indirectly experimental support to the lignin–cellulose interaction.
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Nature Communications
·
2026
·Vol. 17
·期 1
·9594
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IF 18.1
Zhao Peng,Wu Tianwei,Sun Jinsong,Liu Meng,Tang Qi,Ren Zechun,Liu Yongzhuang,Yu Haipeng
The long-standing trade-off between strength and toughness has constrained the performance of thermoplastic elastomers. Here, we address this challenge by constructing a three-dimensional supramolecular network in a thermoplastic polyurethane elastomer via dynamic chain extension with lignin polyols. Unlike conventional linear or branched extenders, lignin’s rigid aromatic backbone and abundant hydroxyl groups serve as multifunctional nodes that simultaneously enhance microphase separation and establish a hierarchical, dynamic hydrogen-bonding network. At an optimal lignin loading of 10 mol%, the resulting material achieves a tensile strength of 127.7 ± 9.52 MPa and a toughness of 1.43 ± 0.11 GJ m⁻³—representing the highest combination reported for polyurethane elastomers to date. In situ spectroscopy and molecular dynamics simulations reveal that lignin transforms the hydrogen-bond landscape from a static binary system into a dynamic, spatially organized architecture, enabling multi-scale energy dissipation through sacrificial bond rupture and subsequent network reorganization. This lignin-engineered network also imparts superior damage tolerance and high elastic recovery to fiber-reinforced composites. This work unveils a general strategy for employing bio-aromatic motifs to effectively decouple the strength-toughness conflict in thermoplastic elastomers, paving the way for high-performance composites.
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INDUSTRIAL CROPS AND PRODUCTS
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2023
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IF 5.9
Rui Tian,Yue Liu,Chao Wang,Weikun Jiang,Srinivas Janaswamy,Guihua Yang,Xingxiang Ji,Gaojin Lyu
In the present work, hollow and solid lignin nanoparticles (LNPs) were synthesized through a self-assembling process using the organosolv pretreatment of lignin from the eucalyptus and willow byproducts. The SEM , TEM, and zeta potential establish the LNPs of a uniform spherical morphology, and the hollow lignin nanoparticles (HLNPs) display the inner cavity and shell. The polyvinyl alcohol (PVA) nanocomposite films containing the LNPs suggest that the presence of HLNPs results in a “room” like network structure in the films and differs from the solid lignin nanoparticles (SLNPs) induced structural changes. The LNPs inclusion increases the mechanical properties. The films with solid eucalyptus lignin nanoparticles showed excellent tensile strength (132 MPa), while those with hollow eucalyptus lignin nanoparticles resulted in exceptional elongation at break (324%). Hydrophobicity tests revealed that both LNPs incorporation in the PVA film results in a water contact angle of more than 90°. The outcome promises novel opportunities for LNPs in the designing and development of plastic replacement packaging films.
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