ACS Sustainable Chemistry & Engineering
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2019
·
IF 6.97
Yuan Liu,Xing Huang,Kaichen Han,Yuhua Dai,Xueqin Zhang,Yuxia Zhao
Developing low-migration macromolecular photoinitiators (macro PIs) is significant to achieve a sufficient biosafety for photopolymers. In this study, for the first time lignin was introduced into photoinitiating systems. A novel lignin-based water-soluble macro PI (L-PEG-2959) was designed and synthesized by introducing water-soluble PEG chain and photoinitiating moiety into lignin backbone simultaneously. A series of characterizations were performed, including 1H NMR, FTIR, UV–vis, GPC, and TGA analysis, which indicated that L-PEG-2959 has excellent light absorption property within 200–400 nm, high initiating efficiency, and superior water solubility. Additionally, L-PEG-2959 could be compatible well with glycidyl methacrylate-modified gelatin (Gel-GMA) and initiate the photopolymerization of Gel-GMA quickly under UV irradiation to form a chemical cross-linking hybrid hydrogel. Compared with the neat hydrogel prepared by Gel-GMA initiated with Irgacure2959, a commercial small molecular PI, the hybrid hydrogels presented controllable swelling property, increased mechanical strength, remarkably reduced precipitates, and enhanced biosafety. The results indicated the great potential of lignin-based macro PIs in preparing biosafety photopolymers.
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CELLULOSE
·
2019
·Vol. 26
·期 4
·2375-2388
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IF 3.917
Zhang Lili,Lu Hailong,Yu Juan,Fan Yimin,Ma Jinxia,Wang Zhiguo
Abstract Lignocellulose hydrogels (LCGs) with varying lignin content were prepared by the dissolution–regeneration process using N -methylmorpholine- N -oxide solvent system. The varying lignin content in LCGs can lead to different aggregation states due to the hydrophobic association of lignin, with an important impact on the micromorphology and pore structure of hydrogel. The presence of lignin is beneficial for the mechanical improvement of LCGs when lignin content is lower than 6.5%. LCGs with 6.5% lignin exhibits better viscoelasticity (580.0 kPa), compressive modulus (55.0 kPa), and a more homogeneous structure than others. The LCGs with a lignin content of 11.6% exhibit the best adsorption property (86.1 mg g −1 for Pb 2+ and 69.3 mg g −1 for Cu 2+ ), which is dominated by chemisorption and multiple diffusion mechanisms. The work provides a feasible route for lignin-containing hydrogel production and develops a method for tailoring micromorphology and the physical properties of the hydrogel by controlling lignin content. Graphical abstract
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Waste and Biomass Valorization
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2019
·Vol. 11
·期 8
·4561-4569
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IF 2.358
Yu Hongfei,Zhan Wang,Liu Yun
Abstract Lignin is the second-most abundant natural organic material after cellulose and the richest aromatic organic biopolymer on earth. It was typically burned for energy generation with low economic benefits. To date, it remains still challenging to valorize lignin with a simple and straightforward strategy in an industrial scale-up. Here, we fabricate two highly hydrophobic melamine sponges with excellent adsorption performance and flame retardancy through a facile spontaneous deposition of lignin and/or acetylated lignin nanoparticles onto the MF sponge skeleton. Two targeted sponges show micro-nano structure with high porosity and robust properties for absorbing oils and organic solvents from contaminated water. Over 85% of the absorbed oils and solvents can be harvested by either batch squeezing way or continuous operating mode with the assistance of constant-flow pump. Interestingly, the targeted sponges exhibit satisfactory flame retardancy property to diminish the risk of fire and explosion when ignited. More importantly, the targeted sponges endorse excellent recyclability and robust stability after 60 repetitions with neglective lignin leaching. It is worthy to point out that the findings in our work opens up a new way for lignin valorization, which is a promising cost-effective and facile scalability processing to fabricate oil/water separation absorbent, since it requires neither hazard modifier agents nor sophisticated equipment. Graphic Abstract
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Journal of Materials Chemistry A
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2018
·Vol. 7
·期 3
·1233-1243
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IF 9.931
Songqi Ma,Jingjing Wei,Zhen Jia,Tao Yu,Wangchao Yuan,Qiong Li,Sheng Wang,Shusen You,Ren Liu,Jin Zhu
Conventional thermosets, widely used in composites, coatings, electronic packing materials, etc., are typically made of non-sustainable fossil resources and cannot be recycled under mild conditions. Degradable thermosets are promising alternatives, while combining ready degradability and high performance is a challenge. In this paper, for the first time, a spiro diacetal structure was utilized to synthesize readily recyclable thermosetting materials with high performance. A renewable bioresource, lignin derived vanillin, was used to produce a rigid spiro diacetal trigger and further built into three thermosets. Among them, spiro diacetal epoxy resin was systematically investigated and was proved to be readily degradable under mild acidic conditions while maintaining stability under neutral or basic conditions and showing outstanding thermal stability. Meanwhile, its glass transition temperature, tensile strength, modulus, elongation at break are comparable to or even better than those of conventional bisphenol A epoxy resin. Moreover, facilely recyclable carbon fiber reinforced composites and convenient-removal coatings were achieved from this epoxy resin accompanied by excellent performances.
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ChemSusChem
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2018
·Vol. 12
·期 4
·944-954
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IF 7.411
Shi Qiu,Xuan Guo,Yong Huang,Yunming Fang,Tianwei Tan
Graphical Lignin first : A flexible lignin-first biorefinery could be developed by task-specific catalyst design for hemicellulose retention or feedstock extension. Mo x C/carbon nanotube (CNT) is found to be a promising catalyst for the retention of hemicellulose by cleavage of the bonds between lignin and carbohydrates with high selectivity. Ru/CMK-3 achieves the extension of the feedstock for the lignin-first biorefinery from hardwood to softwood. A catalytic reductive fractionation method for lignocellulosic biomass, termed lignin-first biorefinery, has emerged, which emphasises preferential depolymerization of the protolignin. However, in most studies, the lignin-first biorefinery is only effective for hardwood that has a high syringyl/guaiacol (S/G) ratio of lignin building blocks, and the degradation of hemicellulose also takes place simultaneously to a certain degree. In this study, two task-specific catalysts were developed to realize hemicellulose retention and feedstock extension through the development of an objective performance–structure relationship. It is found that Mo x C/carbon nanotube (CNT) is highly selective in the cleavage of bonds between carbohydrates and lignin and ether bonds in lignin during the catalytic reductive fractionation of hardwood, leading to a carbohydrate (both cellulose and hemicellulose) retention degree in the solid product close to the theoretical maximum and a delignification degree as high as 98.1 %. Ru/CMK-3 is demonstrated to be effective in the catalytic reductive fractionation of softwood and grass, resulting from its weak acidity and high mesoporosity.
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高影响因子
APPLIED ENERGY
·
2018
·
IF 7.9
Wanwu Li,Habiba Khalid,Zhe Zhu,Ruihong Zhang,Guangqing Liu,Chang Chen,Eva Thorin
Lignocellulosic biomass is the most abundant natural resource with high biomethane potential. However, complex structure of lignocellulosic biomass has hampered the efficient utilization of this bioresource. Previous studies have investigated the overall anaerobic digestion performance of lignocellulosic biomass, but the individual participation of each lignocellulosic component during anaerobic digestion remained unclear. Thus, this study investigated the methane production characteristics of cellulose, hemicellulose, lignin and their mixtures along with the microbial communities involved in anaerobic digestion. The results showed that the biomethane potential of cellulose was higher than that of hemicellulose; however, hemicellulose was hydrolysed more quickly than cellulose, while lignin was very difficult to be digested. The higher concentrations of acetic, n -butyric and n -valeric acids hydrolysed from the hemicellulose resulted in a lower pH and more severe inhibition on methane production than that of cellulose, and the methanogenesis gradually recovered after pH adjustment. The co-digestion of cellulose and hemicellulose increased the methane yield and biodegradability compared to mono-digestions. The addition of lignin to cellulose brought more significant decrease in the methane yield of cellulose than that of hemicellulose. Substrate-related bacteria such as Clostridium sensu stricto , Lutaonella , Cloacibacillus and Christensenella showed higher relative abundance in cellulose digestate, and sugar-fermenting bacteria such as Saccharofermentans , Petrimonas and Levilinea were more rich in the digestate of hemicellulose. Moreover, methanogenic Methanospirillum and Methanothrix likely contributed to the methane production of cellulose, while aciduric methanogens from Methanobrevibacter , Methanomassiliicoccus , Methanobacterium and Methanoculleus contributed to that of hemicellulose. This study provides a deeper understanding of the mechanism in the bioconversion of lignocellulosic biomass during anaerobic digestion.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2019
·
IF 4.784
Chao Xu,Jun Zhang,Yu Zhang,Ying Guo,Huijuan Xu,Cuiyi Liang,Zhongming Wang,Jingliang Xu
Sugarcane bagasse (SCB) was pretreated by sodium hydroxide (SH), alkaline ethanol (AE) and alkaline hydrogen peroxide (AHP), and the solid residue with similar lignin content after different pretreatment was selected. Enzymatic saccharification with different substrates was performed at 2%, 10%, and 20% ( w / v ) solid loading. After that, the lignin from different substrate was extracted and its structure was characterized. Furthermore, the adsorption capability of isolated lignin to cellulase and its effect on enzymatic hydrolysis were studied. The results showed that, as the substrate content increased from 2% (w/v) to 20% (w/v), the glucose yield after digestion of SH, AE, and AHP pretreated SCB reduced by 41.8%, 35.4%, and 28.7%, respectively. The inhibitory effect of different prepared lignin on the digestibility of Avicel was as follows, SH pretreated lignin (SHL) > cellulase enzymatic hydrolysis lignin (CEL) > AE pretreated lignin (AEL) > AHP pretreated lignin (AHPL), which exhibited positive correlation with its non-productive adsorption capability to cellulase. Lignin samples with low negative zeta potential , high hydrophobicity and high ration of syringyl (S) to guaiacyl (G) were unfavorable for the enzymatic saccharification of cellulose .
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Journal of Cleaner Production
·
2024
·
IF 9.7
Yang Liu,Chunbao Zhou,Asif Ali Siyal,Chenglong Liu,Yingwen Zhang,Jie Fu,Huimin Yun,Jianjun Dai,Xiaotao Bi
In this paper, a cleaner pyrolysis strategy combining microwave heating, catalyst and carbon dioxide was explored for converting biomass components into higher quality products. Catalytic pyrolysis was more favorable for the decomposition and conversion of complex biomass structures. For furfural residue pyrolysis , potassium sulfate contained in sample served as the main catalytic component. Potassium sulfate promoted the increase of phenols in bio-oil. Notably, carbon dioxide atmosphere promoted the decomposition of substances and exerted a significant effect on biomass pyrolysis , which increased bio-oil yield and declined gas yield. When the pyrolysis atmosphere was changed from nitrogen to carbon dioxide, the I D /I G ratio decreased from 1.07 to 0.74, indicating that carbon dioxide decreased defect structure in biochar. Carbon dioxide enriched the porous structure and surface roughness of biochar. Also, carbon dioxide as a carrier gas was found to be more effective than nitrogen in improving the heating values of biochar and the acidity of bio-oil under carbon dioxide was lower than that under nitrogen, which was conducive to the subsequent utilization of biochar and bio-oil. Carbon dioxide promoted the production of alcohols, alkenes , and alkanes in bio-oil. Beneficially, the interaction of cellulose and lignin inhibited the release of hydrogen chloride . At last, this study also provides insights into the mechanism of catalyst and CO 2 on biomass microwave pyrolysis .
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GREEN CHEMISTRY
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2024
·
IF 9.3
Zuzhi Li,Ya Ma,Xingjie Guo,Yang Cao,Qian Jiang,Mi Gao,Xudong Liu,Daniel C. W. Tsang,Zhicheng Jiang,Bi Shi
Efficient catalytic hydrogenation of lignin-based derivative vanillin (VAN) into valuable chemicals with a high selectivity is important yet challenging because of the lack of selective and active catalysts. Herein, a mixture of polyacrylonitrile (PAN) and water-insoluble tannin (Tan) was employed to create composite fibers through the electrospinning process, resulting in PAN–Tan composite fibers. The formation of hydrogen bonds between the –CN group of PAN and the phenolic –OH group of Tan proved advantageous for high dispersion and reduced physical entanglement, resulting in the production of thinner fibers. Leveraging abundant ortho-phenolic –OH groups of Tan, the PAN–Tan fibers were used to adsorb Pd2+ ions, which were reduced by in situ reduction process to Pd0 particles. Higher solute concentrations in the spinning solution improved the homogeneity of the electrospun PAN–Tan fibers, facilitating the dispersion and reduction of adsorbed Pd2+ on the fiber surface. Subsequently, these Pd/PAN–Tan fibers served as catalysts for the selective hydrogenation of the –CHO group of VAN to produce vanillyl alcohol (VAL) in an aqueous phase. Over 99% of VAN could be hydrogenated into VAL at 50 °C for 60 min under 0.5 MPa H2. Moreover, the catalyst exhibited universal applicability for the hydrogenation of diverse typical lignin-based aromatic aldehydes. The catalytic hydrogenation of VAN was then extended to a fixed-bed reactor for 24 h, and only VAL was detected in the effluent. Our study underscored the low energy consumption for catalyst preparation without additional reducing agents and high temperature carbonization process, the stability and reusability of the Pd/PAN–Tan fiber catalyst and its potential for large-scale industrial applications.
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BIORESOURCE TECHNOLOGY
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2024
·
IF 9.7
Ziyu Jia,Jun Hu,Ping Lu,Yunjun Wang
Carbon quantum dots (CQDs) were successfully synthesized from carbohydrate-rich residue of birch obtained following the lignin-first strategy. The optical and physicochemical properties of the CQDs were studied, along with their potential for photocatalytic pollutant degradation. By combining solvothermal and chemical oxidation methods, the product yield of CQDs from carbohydrate-rich residue reached 8.1 wt%. Doping nitrogen enhances the graphitization of CQDs and introduces abundant amino groups to the surface, thereby boosted the quantum yield significantly from 8.9 % to 18.7 %-19.3 %. Nitrogen-doped CQDs exhibited efficient photocatalytic degradation of methylene blue, reaching 37 % within 60 min, with a kinetic degradation rate of 0.00725 min −1 . This study demonstrates that carbohydrate-rich residue obtained from lignin-first strategy are ideal precursors for synthesizing CQD with high mass yield and quantum yield by combining solvothermal treatment and chemical oxidation methods, offering a novel approach for the utilization of whole biomass components following the lignin-first strategy.
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CHEMICAL ENGINEERING SCIENCE
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2024
·
IF 4.1
Fenghao Shu,Guangcai Long,Yanwu Chen,Ying Gao,Menghao Jiang,Jinxing Long
Conversion of renewable lignin to value-added aromatic chemicals presents a broad prospect to achieve the goals of “carbon neutrality”. In this work, an efficient approach is proposed for selective hydrogenolysis of lignin to valuable 4-propyl syringol in the presence of cost-effective catalyst of y Ni/ZrO 2 - x MoO 3 . When the lignin hydrogenolysis is performed with 15Ni/ZrO 2 -10MoO 3 , 15.4% yield of monophenols is achieved, which is approximately twice as that from the 15Ni/ZrO 2 catalytic system (7.8%). Importantly, 33.1% of these monophenols are identified as 4-propyl syringol (4-PS), a versatile fine chemical. An extensive characterization of the modified catalysts by means of XRD, nitrogen adsorption–desorption isotherm, SEM, TEM, XPS, NH 3 -TPD, CO 2 -TPD, and H 2 -TPR, confirms that the introduction of MoO 3 changes the primary phase of ZrO 2 and the acidity/basicity properties of catalyst. As a result, an enhanced cleavage of the C-O linkage between S-lignin and other units is demonstrated, which consequently contributes to the good selectivity of 4-propyl syringol. Therefore, this work provides a new insight for producing bulk aromatic chemicals via a sustainable route.
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BIORESOURCE TECHNOLOGY
·
2012
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IF 4.98
Long Lin,Shang-Ru Zhai,Zuo-Yi Xiao,Na Liu,Yu Song,Bin Zhai,Qing-Da An
A simple method to the preparation of SiO 2 microspheres from rice husks (RH) was developed. The rice husks were extracted with 2 M NaOH solution to obtain a extract contained silica and lignin, and silica spheres were obtained after addition of distilled water, ethanol, 1 M H 2 SO 4 and PEG (W silica :W PEG = 2:1) to the extract in a controllable sol–gel process and calcination at 550 °C. The optimum synthesis conditions were, adjustment of the extract to pH 3, a volume ratio of 1:1:2 of ethanol, water, and extract, respectively and a silica to polyethylene glycol weight ratio of 2:1. The SiO 2 microspheres produced under these conditions exhibited a relatively uniform particle size distribution around 500 nm as determined by LPSA, which indicated a cooperative function of added PEG and extracted lignin towards the formation of SiO 2 microspheres.
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高影响因子
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