INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
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IF 6.953
Ze Yuan,Xinyue Shang,Jing Fang,Hao Li
The waterborne polyurethane (WPU) exposed to outdoor environment for a long time are more likely to reduce their mechanical performance and service life. This work describes a simple and effective method to obtain the homogeneous lignin/TiO 2 nanocomposite as the anti-UV additive to improve the applicability of WPU. The SKLs/TiO 2 were prepared by the gradient sulfonation kraft lignin (SKLs) and tetrabutyl titanate. The particle morphology and hybrid structure of SKLs/TiO 2 are characterized by FT-IR, zeta potential analysis, XPS, TG and SEM. Interestingly, it was found that the change of π-π interactions and electrostatic repulsion between SKL molecules effected the forming of SKLs/TiO 2 nanocomposite. The lignin content and morphology of SKLs/TiO 2 nanocomposite could be controlled by regulating the sulfonate group content on lignin molecular. Furthermore, the SKLs/TiO 2 nanocomposites was successfully applied on water polyurethane film as the additive, when SKLs/TiO 2 content increased from 0 wt% to 5.0 wt%, the tensile strength increased 43%, the elongation at break increased from 240.0% to 352.0% and the UV transmittance reduced from 87% to 1.7% below 400 nm, which greatly improved the UV resistance and mechanical properties. The results of this study are of significant and practical importance to the high-value-added utilization of lignin.
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Journal of Energy Chemistry
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2023
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IF 13.1
Zhe-Hui Zhang,Xianyuan Wu,Xiaohong Ren,Zeming Rong,Zhuohua Sun,Katalin Barta,Tong-Qi Yuan
Transformation of lignin to valuable chemicals via sustainable pathways is recognized as one of the most efficient ways to explore its value and replace the nonrenewable petroleum resource. In this work, an environmental-friendly transfer hydrogenation process has been developed to convert lignin derived 2,6-dimethoxybenzoquinone to 1,4-cyclohexanediol. Compared with previous work under hydrogen pressure (30 bar), this process uses isopropanol as both solvent and hydrogen donor, which significantly simply the operation process. The core of this study is the design and preparation of Mn modified Raney Ni catalysts by ball milling process. A series of Raney NiMn catalysts with different ball milling time and Mn content were prepared and investigated. Characterizations by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM) and transmission electron microscope (TEM) etc. showed that NiMnAl alloy was formed during the ball milling process and then transformed to NiMn alloy after treatment by aqueous NaOH. After optimization, a yield as high as 86.1% could be achieved for 1,4-cyclohexanediol at 200 °C in only 1 h.
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ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Xiangchen Kong,Chao Liu,Yuyang Fan,Ming Li,Rui Xiao
The conversion of crude lignin bio-oil to jet fuels is a highly desirable target for biorefineries, especially in light of the global energy crisis. The key to achieving this goal is the realistic tuning of catalyst efficiency and selectivity for expected products. Herein, a copper catalyst with enhanced activity for hydrodeoxygenation (HDO) of crude lignin bio-oil to jet fuel precursors was developed in this work. The copper catalyst, a copper-doped porous metal oxide, was modified with a series of moderate organic acids to graft the acidic O-groups as potential Brønsted acid sites for HDO reactions. The copper catalyst modified with propanoic acid exhibited exceptional catalytic performance for the upgrading of lignin pyrolysis bio-oil, giving yields of jet fuel precursor range cycloalkanes and cycloalcohols of 10.04 and 14.20 C%, which were improved by 88.0 and 42.7% compared with those from the blank. Meanwhile, the corresponding hydrogenation and deoxygenation degrees of the products reached 91.5 and 65.9%, respectively, which were improved by 17.3 and 31.8%. Likewise, the overall double bond equivalence and aromaticity index of the products given by the modified copper catalyst were as low as 2.8 and 0.1, which were substantially reduced by 18.0 and 50%, correlating to higher HDO efficiency. The abundant Brønsted acid sites with proper strength and the affluent pore structures of the propanoic acid-modified copper catalyst mainly contributed to its outstanding catalytic activity. The findings suggest promising avenues for increasing the efficiency of heterogeneous catalysts in the HDO of lignin-based bio-oil to alternative fuels.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Qianqian Tang,Hao Wu,Mingsong Zhou,Dongjie Yang
Presently, most studies on modified lignin focused on the adsorption to heavy metal cations, but rarely to Ca 2+ in hard water . Therefore, this work prepared a new gel-type lignin-based cationic adsorption resin (E-LSAF) through the crosslinking and curing of alkali lignin grafted by sodium sulfite sulfonated acetone to remove Ca 2+ in water. Under the determined optimum synthesis conditions, E-LSAF with a highest sulfonic group content of 1.99 mmol/g was obtained. Structural and physicochemical measuring results showed E-LSAF was a gel-type resin, owning strong hydrophilicity , high mechanical strength, excellent thermal stability and acid-alkaline resistance. Adsorption results indicated the adsorption of E-LSAF to Ca 2+ was well-fitted by Langmuir model, and the maximum adsorption capacity reached 45.8 mg/g. Pseudo-second-order model can describe this adsorption process well, suggesting it a chemisorption process. Dynamic column adsorption results showed E-LSAF could transform hard water into soft or even very soft water. The regeneration efficiency still maintained 80 % after 5 cycles. The adsorption mechanism was attributed to electrostatic attraction, ion exchange and complexation. This work provided a high-performance lignin-based cationic adsorption material with high adsorption capacity to Ca 2+ and excellent acid-alkaline resistance, which filled the research gap of using modified sulfonated lignin to remove Ca 2+ from water.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xinpeng Che,Meiyan Wu,Guang Yu,Chao Liu,Huanfei Xu,Bin Li,Chaoxu Li
Flexible actuators with responses to various environmental stimuli have attracted great attention, but the issues of weak layer-to-layer bonding and low water resistance of cellulose-based actuators severely restrict their practical application. Herein, inspired by the internal structure of lignocellulose and reversible opening movement of pine cones by external humidity stimuli, a novel Janus film consisting of the insulated lignin-containing cellulose nanopaper (CNP) layer and the conductive reduced graphene oxide (rGO) layer was delicately designed and well fabricated through lignin adhesion between the two layers. Characterization showed that the obtained Janus film with a tensile strength of 141 MPa could be used as a flexible actuator, which could be operated based on water absorption and dehydration of the CNP layer as well as the light-to-heat conversion and high conductivity of rGO layer. Thus, the as-fabricated Janus film with excellent durability (folding resistance (>1000 times), good wet stability, and durable electrical actuation (>500 cycles)) had quick multi-responses to humidity, near-infrared radiation and electrical stimulation. Particularly, the resultant Janus film had the fastest response speed (1.875°/s/V) under the electrical stimuli compared to the reported carbon/polymer-based flexible actuators with comparable weights. Therefore, this CNP-based Janus film can be potentially used in many fields such as humidity sensor, bionic artificial arm/driving motor, and it could be helpful to develop facile and environmentally friendly strategies for the construction of multi-responsive Janus actuator/intelligent devices.
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Sustainable Energy & Fuels
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2021
·Vol. 5
·期 23
·6097-6106
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IF 6.367
Bowen Luo,Zhixiang Huang,Riyang Shu,Yu Cheng,Zhipeng Tian,Chao Wang,Ying Chen
A lignin-first strategy is promising in lignin utilization to produce value-added aromatic compounds and their derivatives for achieving high efficiency. In this work, we explored the hydrogenolysis of cornstalk lignin in supercritical ethanol and investigated the effects of metal sites and acid sites during lignin-first fractionation. By comparison, the acid pretreatment of Ru/C catalysts significantly promotes the hydrogenolysis process, wherein Ru/C-acid (10) exhibits the best result with 42.9 wt% yield of monomer products (including aromatic monomers and hydrogenated monomers) at 260 °C, 3 MPa H2 for 4 h. Catalysts were measured by BET, TEM and NH3-TPD characterizations, and the hydrogenolysis products were compared by GC-MS, GPC, element analysis and FT-IR characterizations. The analysis results indicate that the active metal site and the abundant acid site are mainly responsible for the efficient lignin hydrogenolysis performance, and these two factors present a significant effect to achieve a high monomer yield.
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ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Haohan Wu,Yingchun Liu,Liheng Chen,Zhengwen Li,Zhaosong Hu,Xuliang Lin,Xueqing Qiu
Enhancing the interface compatibility between the polymer matrix and filler is still a hotspot issue for the fabrication of thermal management materials. In this work, biomass lignin was used innovatively as coupling reagents to optimize the interface microstructure of the matrix/filler. The as-prepared lignin-graphite (AL@GP) and epoxy resin with a Schiff base structure (PBD-EP) were employed as functionalized filler and polymer matrix, respectively. And a degradable and thermally conductive epoxy composite was prepared through the hot-press technique. Experimental and theoretical calculations results based on the first principles demonstrated enhanced interface bonding between GP and PBD-EP. Besides, the developed polymeric composites exhibited excellent thermal conductivity (2.852 W m–1 K–1) when loaded with 50 wt % AL@GP, increasing by 26.1% compared with the PBD-EP/GP system. Moreover, it presented a reduced interface thermal resistance (0.10745 m2 K W–1) and superior solvent-free green degradability. LED heat dissipation experiments indicated the potential of as-prepared composites for thermal management applications. This work not only provides a novel and facile filler functionalization strategy for improving the interfacial interaction of the matrix/filler but also promotes the high-value applications of biomass lignin.
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CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Zeyu Niu,Xin Huang,Tianlong Liu,Yunlin Shao,Chuan Ma,Jingyu Ran
Hemicellulose and lignin decreased the activation energy of cellulose pyrolysis by 36.7 and 22.6 kJ/mol. • Hemicellulose interacted cellulose decreased levoglucosan yield by up to 34-fold due to volatile-acid scission. • Lignin interacted cellulose enhanced levoglucosan yield by up to 77% due to thermal ejection and radical stabilization. Understanding the interactions between biomass components during pyrolysis is crucial for product control. Here, we employed a selective graded decoupling strategy to construct cellulose-hemicellulose (C-H) and cellulose-lignin (C-L) binary systems with varying ratios from pine as a typical woody biomass. Fractionation altered sample morphology from dense to porous, yet cellulose I crystallinity was retained in all samples. The effects of varying hemicellulose and lignin contents on cellulose pyrolysis were studied by thermogravimetric analysis coupled with Fourier transform infrared spectroscopy (TG-FTIR), pyrolysis–gas chromatography/mass spectrometry (Py-GC/MS), and kinetic analysis. The distributed activation energy model (DAEM) study showed that interactions with hemicellulose and lignin decreased the activation energy of cellulose pyrolysis by 36.7 and 22.6 kJ/mol, respectively. C-H interaction promoted the early evolution of CO 2 and carbonyl compounds, whereas C-L interaction enhanced the release of aromatic phenols while inhibiting the generation of hydrocarbons. C-H interaction drastically reduced levoglucosan (LGA) yield by up to 34-fold and shifted products toward small oxygenates possibly due to the random bond scission catalyzed by hemicellulose-derived acidic volatiles. In contrast, C-L interaction increased the yields of LGA and phenolic compounds by 77% and 70%, respectively. The increase in LGA may be due to a lignin-induced thermal ejection effect that facilitates its rapid escape, while the phenolic enrichment may involve radical stabilization by cellulose-derived hydrogen donors. This study reveals the distinct effects of hemicellulose and lignin on cellulose pyrolysis with biomass, providing a theoretical basis for selective valorization of lignocellulosic biomass. Download: Download high-res image (162KB) Download: Download full-size image
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
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IF 6.1
Ye Tian,Ye Yuan,Bing Yuan,Fengli Yu,Congxia Xie,Shitao Yu
The conversion of lignin-based platform compounds into valuable biofuels and chemicals through catalytic processes is an attractive approach for the efficient valorization of renewable lignocellulosic biomass. One such process is the hydrodeoxygenation (HDO) of lignin-based vanillin (VL) to produce 2-methoxy-4-methylphenol (MMP), which is a promising liquid fuel and intermediate for fine chemicals. However, the development of a cost-effective catalytic system with high activity and selectivity remains a challenge. In this study, we report the preparation of a highly-efficient magnetic Co nanoparticles catalyst, CoZn@N-ALC, using alkali lignin as an assembly macromolecular ligand, Zn as a sacrificial metal, and dicyandiamide as a nitrogen source before the pyrolysis process. Various characterization techniques, including powder X-ray diffraction (XRD), pyridine adsorption infrared spectroscopy (Py-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), isothermal nitrogen adsorption/desorption, and X-ray photoelectron spectroscopy (XPS), were employed to investigate the role of zinc and nitrogen in the construction process of CoZn@N-ALC and the influence of catalyst preparation conditions. The optimized CoZn@N-ALC catalyst demonstrated nearly 100 % conversion of VL, complete selectivity towards MMP, and easy separation from the aqueous HDO system. Structure-performance investigation and density functional theory (DFT) calculations suggest that the exceptional catalytic performance of this catalyst can be attributed to the selective adsorption of C=O bonds by abundant Co (1 1 1) active species and its Lewis acid sites. This work provides valuable insights into the rational design of efficient, non-noble metal nanoparticle catalysts based on alkali lignin for the conversion of lignin-based platform compounds.
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CARBOHYDRATE POLYMERS
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2023
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IF 11.2
Jiajun Feng,Yuxian Xing,Chuantao Yin,Pengfei Tang,Feng Jiang
Sustainable elastomers derived from renewable biobased resources with excellent mechanical properties and varied functions are highly pursued to substitute traditional petroleum-based polymers yet challenging due to their limited macroscopic performance. In this work, we designed a series of wholly biobased cellulose- graft -poly(vanillin acrylate- co -tetrahydrofurfuryl acrylate) (Cell- g -P(VA- co -THFA) copolymer elastomers with cellulose as the rigid backbone, sustainable VA derived from lignin and soft THFA derived from hemicellulose as the hard and soft segments in the rubbery side chains. Moreover, the grafted side chains can be cross-linked to introduce an additional dynamic network structure via Schiff-base chemistry between the aldehyde and amino groups. The mechanical properties of Cell- g -P(VA- co -THFA) copolymer elastomers, including tensile strength , extensibility, elasticity, and toughness can be facilely manipulated by the VA/THFA feed ratio, cellulose content, and cross-linking density. These Cell- g -P(VA- co -THFA) copolymer elastomers are thermally stable and possess outstanding adhesion behavior and prominent UV-shielding performance. Besides dramatically enhanced mechanical properties, the cross-linked Cell- g -P(VA- co -THFA) counterparts exhibit remarkable shape memory behavior. This work provides a robust and convenient strategy for developing strong and versatile sustainable elastomers with different application demands by integrating different biomass feedstocks via elaborate molecular design.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Shuai Ding,Yanchen Zhu,Haonan Zhang,Yajun Fu,Hao Ren,Huamin Zhai
Cr (VI) accumulates in an aqueous environment and exhibits huge harm to human health and the ecological system. Developed lignin biomass materials are complicated to prepare and have limited properties, and advances in lignin phenolic modification are lacking. Herein, an aminated poplar lignin-pyrogallol (PLP-PEI) with a simple design and adjustable phenolic hydroxyl content was developed using the acid hydrolysis-phase separation (AH-PS) method, and modified by the atom transfer radical polymerization (ATRP) strategy. Through diverse characterization analysis, the structural changes of PLP-PEI in the step-by-step synthesis process were monitored. An effective biomass capture system (Bio-Cap) was shown via systematically investigating the adsorption behaviors of Cr (VI) on PLP-PEI under various environmental conditions. Benefiting from introducing phenolic hydroxyl and amino groups, PLP-PEI demonstrated efficient adsorption capacity (598.80 mg/g for Cr (VI)). Additionally, the material also exhibited advantages, including monomeric chemisorption properties, strong reduction capability, and stable regeneration properties. Multiple driving forces were involved in the capture and removal process of Cr (VI), including complexation and electrostatic interaction. The low-cost natural biomass resources supported the industrial-scale synthesis and practical application of advanced aminated lignin polyphenol material, which showed outstanding advantages and enormous potential in the field of water environmental restoration.
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FOOD HYDROCOLLOIDS
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2023
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IF 10.7
Shikai Zhang,Quanbin Fu,Houshen Li,Yijing Li,Peng Wu,Shiyun Ai
The potential of polysaccharide film as an alternative to petroleum-based plastics is being closely watched. To solve the defects of poor water resistance, poor flexibility and no bioactivity of polysaccharide-based films, polydopamine-coated lignin nanoparticles (LNP@PDA) were prepared and loaded on polysaccharide matrix to obtain composite films. LNP@PDA has good biocompatibility and can be dispersed homogeneously in polysaccharide matrix. The tight entanglement and hydrogen bonding between LNP@PDA and pectin promoted the formation of dense structure in film, and allowed the films to exhibit a nano-scale rough surface (7.61–20.90 nm). Composite films have higher mechanical strength (35.76 MPa) and water contact angle (92.42°), and exhibit unique antioxidant and antibacterial activities. Even without the addition of any plasticizers, the composite film exhibits attractive flexibility that is not present in polysaccharide-based films. When LNP@PDA loading exceeded 5%, composite films almost completely blocked the UVA (400-320 nm), UVB (320-275 nm) and UVC (275-200 nm) spectra and remained so after 24 h of UV irradiation, which demonstrated their excellent UV resistance and photostability. Furthermore, the universality results verify that LNP@PDA is also suitable for other different polysaccharide-based (such as starch , sodium alginate , agar, carrageenan , carob gum) films. Interestingly, the shear-thinning property of the film-forming fluid allows it to be sprayed through a sprayer bottle onto the surface of fruit or food packaging. These results suggest that LNP@PDA can be loaded into polysaccharide-based films as plasticizers, mechanical property enhancers, anti -UV agents, antioxidants and antimicrobial agents. This provides a brand-new strategy for producing high-performance polysaccharide-based food active packaging/coating.
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