CARBOHYDRATE POLYMERS
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2022
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IF 10.723
Xiaoyan Yin,Tingting Cai,Chao Liu,Yan Ma,Jun Hu,Jianchun Jiang,Kui Wang
Biorefinery plays a pivotal role in biomass economy with environmentally benign process. Herein, we report a coupling dihydrolevoglucosenone and aqueous p -toluenesulfonic acid (Cyrene/TsOH aq.) system for efficient saccharification of moso bamboo. More than 87.3 % of cellulose recovery could be observed under mild condition of 120 °C for 60 min, accompanied by 85.5 % hemicellulose removal and 79.4 % lignin extraction, respectively. Notably, 90.6 % of saccharified yield could be obtained including 67.7 % of oligosaccharide and 22.9 % of monosaccharide . Besides, the yielded lignin exhibited high purity of 99.1 % and outstanding uniform polydispersity index of 1.49 with nanoscale particle size around 347 nm, which is of great significance for further application. Furthermore, the synergistic effect between Cyrene and TsOH on efficiency and specificity of biorefinery was proposed by control experiments and verified by molecular dynamics simulation and quantum chemical calculation , which provided a new insight for full components biorefinery of lignocellulosic biomass.
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高影响因子
Journal of Environmental Chemical Engineering
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2021
·
IF 5.909
Bin Yan,Xiaoyu Wang,Xiaoling Zhang,Shengqu Liu,Min Li,Rong Ran
Chemical dispersants are a controversial solution for oil spill remediation, and the potential toxicity of chemical surfactants to the marine ecology has prompted much research for eco-friendly dispersants with superior dispersing ability. Herein, an efficient Pickering emulsifier was prepared on the basis of the synergistic effect of sulfonated lignin (SL) and nickel hydroxide (Ni(OH) 2 ) micron particles. The interaction of SL and Ni(OH) 2 particles was characterized by the contact angle, shear viscosity and Zeta potential measurements. Confocal fluorescence microscopy and optical microscopy images revealed the oil droplet structure. The average emulsion droplet size and emulsification index were investigated. These results indicate that the addition of SL has a synergistic stabilizing effect in high salinity seawater. Here, Ni(OH) 2 particles alone are not an efficient emulsifier in seawater because of the strong flocculation caused by high salinity. The adsorption of Ni(OH) 2 particles by SL changed their contact angle and benefitted their adsorption at the oil-seawater interface, providing a solid barrier to avoid droplet coalescence, and the stable O/W emulsion exhibited great stability, smaller droplet size and larger oil-water interface area, which facilitated the subsequent natural degradation of crude oil. Therefore, this may be an environmentally friendly and harmless new method for SL and Ni(OH) 2 particles to deal with marine oil spill problems.
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LANGMUIR
·
2021
·
IF 3.882
Kai Chen,Shengrong Yuan,Dan Wang,Yinli Liu,Fengfeng Chen,Dongming Qi
Avermectin (AVM) is a highly effective and safe biopesticide but is very sensitive to ultraviolet (UV) light and exhibits poor water solubility. Developing green and multifunctional adjuvants is important for the protection and controlled release of AVM. In this work, a number of water-soluble enzymatic hydrolysis lignins (W-EHLs) were prepared via grafting basic amino acids and used as emulsifiers with co-surfactants to prepare high-internal phase emulsions (HIPEs). The results showed that W-EHLs with co-surfactants could be prepared with HIPEs that contained 90 vol % green oil phases such as turpentine, and the stability of the HIPEs first increased and then decreased when the rate of grafting of basic amino acids on lignin increased from 0.26 to 1.46 mmol/g. The more polar oil droplets were less deformable due to their higher viscosity, thereby affording a stability advantage to HIPEs. Subsequently, the relations between the stability and interfacial viscoelasticity of the emulsion were effectively correlated by interfacial rheology, droplet size, and physical stability tests. The results showed that HIPEs with smaller droplets had poor fluidity and strong interfacial viscoelasticity due to their higher droplet packing density, which resulted in good macroscopic stability. Like the AVM carrier, the retention rate of AVM in HIPEs was 80.1% after UV radiation for 72 h, which represented the highest UV protection efficiency in AVM delivery systems. The release curves showed that the rate of release of AVM from HIPEs was adjusted by controlling the pH value of the medium. In addition, the release of HIPEs is completely in accord with both diffusion and the matrix erosion mechanism. The strategy could be extended to other sensitive pesticides and used to promote the development of sustainable agriculture.
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Molecular Catalysis
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2021
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IF 5.062
Changcheng Shen,Wenzhi Li,Baikai Zhang,Fengyang Xue,Xiaomeng Dou,Xia Zhang,Yihang Jiang
Lignin, which represents the most abundant renewable aromatic biomass resource on the earth, is promising as an alternative for the production of chemicals. We presented a modified method that provides the hydrogen source in the reaction with a mixed solvent of alcohol, acid and water, replacing the original method that directly provides a hydrogen source with external hydrogen. In addition, a new cobalt supported on nitrogen doped carbon catalyst preparation method (one-pot) was presented. We proposed one-step method in which corn stover lignin is converted to target monomers over Co/AC-N_one-pot catalyst and mixed solvent. The role of the alcohol to acid and water mixed solvent not only extract lignin fragments from the matrix but also provide the hydrogen source. Cobalt which has electronic interaction with the nitrogen reformed alcohols to obtain hydrogen and stabilized lignin intermediates during the reaction by hydrogenation of active bonds. Different kinds of nitrogen including pyridinic and pyrrolic nitrogen functional groups plays a critical role in stabilizing Co. Nearly complete delignification (91%) and high yield of target monomers (23.8%) can be obtained under the conditions (5wt% Co/Ac-N_one-pot, 10:1:1mixture solvent consist of isopropanol/water/ formic acid , 235 °C, 200 min, 0.1 MPa N 2 ), and the selectivity of target monomers was 85%. Circulation experiment of catalyst was performed directly without any operation of the residue, and it could maintain 90% activity in the first four cycles.
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MOLECULES
·
2021
·Vol. 26
·期 19
·5740
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IF 4.412
Kai Zhang,Yanchao Liu,Sheng Cui,Yimin Xie
To elucidate the chemical linkages between lignin and carbohydrates in ginkgo cell walls,13C-2H-enriched cell wall-dehydrogenation polymers (CW-DHP) were selectively prepared with cambial tissue fromGinkgo bilobaL. by feeding D-glucose-[6-2H2], coniferin-[α-13C], and phenylalanine ammonia-lyase (PAL) inhibitor. The abundant detection of13C and2H confirmed that D-glucose-[6-2H2] and coniferin-[α-13C] were involved in the normal metabolism of ginkgo cambial cells that had been effectively labelled with dual isotopes. In the ginkgo CW-DHP, ketal and ether linkages were formed between the C-α of lignin side chains and carbohydrates, as revealed by solid state CP/MAS13C-NMR differential spectroscopy. Furthermore, the DMSO/TBAH ionic liquids system was used to fractionate the ball-milled CW-DHP into three lignin-carbohydrate complex (LCC) fractions: glucan–lignin complex (GL), glucomannan–lignin complex (GML), and xylan–lignin complex (XL). The XRD determination indicated that the cellulose type I of the GL was converted into cellulose type II during the separation process. The molecular weight was in the order of Ac-GL > Ac-GML > XL. The13C-NMR and1H-NMR differential spectroscopy of13C-2H-enriched GL fraction indicated that lignin was linked with cellulose C-6 by benzyl ether linkages. It was also found that there were benzyl ether linkages between the lignin side chain C-α and glucomannan C-6 in the13C-2H-enriched GML fraction. The formation of ketal linkages between the C-α of lignin and xylan was confirmed in the13C-2H-enriched XL fraction.Keywords:lignin–carbohydrate complexes;CW-DHP;isotope labelling;ginkgo;NMR
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INDUSTRIAL CROPS AND PRODUCTS
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2021
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IF 5.645
Junxian Xie,Jun Xu,Zheng Cheng,Shiyun Zhu,Bin Wang
In this study, the eco-friendly heteropoly acids-phosphotungstic acid (PTA) was chosen as a catalyst to assist neutral deep eutectic solvents (DESs) for deconstructing corn straw. The reactions were performed with a shorter time at 110–150 °C than other DES system. The results revealed that most of the lignin (86.1 %) and hemicellulose (89.7 %) were removed while cellulose was obtained in high yields (88.9–94.3 %). Benefiting from the removal of hemicellulose and lignin, the enzymatic digestibility of pretreated materials was noticeably boosted to 94.4 %, which was 5.3-fold higher than the untreated corn straw. Meanwhile, the regenerated lignin nanoparticle was acquired with a relatively high purity (more than 85 wt%), low and homogeneous molecular weight (5669−2437 g/mol). Furthermore, the PTA/DES demonstrated excellent cycle performance. Overall, technically feasible PTA catalyzed DES pretreatment presented in-depth analysis for effective deconstruction of corn straw recalcitrance for crops valorization in the future.
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RSC Advances
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2021
·Vol. 11
·期 60
·37932-37941
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IF 3.361
Ge Guo,Wenzhi Li,Tauseef Ahmed,DuoDuo Hu,Ru Cui,Baikai Zhang,Xia Zhang
Non-noble bimetallic NiMo supported on zeolitic imidazolate framework-derived porous carbon (NiMo@FDC) catalyst for lignin depolymerization has been successfully developed. The synergism between Ni and Mo species in NiMo@FDC catalyst could promote the catalytic cleavage of C–O linkages in Kraft lignin. At a low reaction temperature of 240 °C and under 4 MPa H2, the lignin liquefaction yield was 98.85 wt% and minimum coke yield was 1 wt%, particularly when using 10%NiMo@FDC catalyst. Additionally, at a high reaction temperature of 300 °C and under 2 MPa H2, there was an overall yield of 86 wt% of liquid product and 42 wt% of petroleum ether soluble product. The higher heating value (HHV) increased from 27.65 MJ kg−1 to 34.11 MJ kg−1. In the cycling experiment, the bifunctional catalyst also demonstrated reversability and stability. The synergy of Ni hydrogenation sites and Mo coupled adsorption sites identified a possible mechanism path, which could offer considerable potential for lignin depolymerization.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Lang Gong,Hongye Wu,Xiangyi Shan,Zhili Li
The development of low-cost, high-efficienct, and environmentally benign adsorbents for the removal of antibiotics and heavy metal ions in water is greatly needed. Phosphorylated alkali lignin (PAL) microparticles were newly fabricated via a facile one-pot method. The characterization confirmed that the phosphate group was successfully introduced into the lignin matrix, and the specific surface area of the obtained PAL was 9.53 m 2 ·g -1 , 5.6 times that of lignin (1.71 m 2 ·g -1 ). The adsorption behavior of PAL was initially investigated in a batch mode by using levofloxacin hydrochloride (LH) as a model. PAL performance was then validated to other contaminants as Pb(II), tetracycline (TC), and sulfadiazine (SA). The results indicated that 99.91% of LH ( C 0 =80 mg·L -1 ) could be removed by PAL (0.02 g/50 mL) within 80 min. The adsorption capacity of PAL to LH and Pb(II) reached 389.1 mg·g -1 and 349.2 mg·g -1 , respectively, better than earlier adsorbents. Importantly, PAL had a strong ability to remove the complex pollutants with coexisted Pb(II) and LH in water and was also applicable for adsorption of TC and SA. XPS and FTIR results show that the adsorption is mainly related to π-π stacking, hydrogen bonds and electrostatic interaction. The adsorption amount of LH in fixed-bed column was 240.5 mg·g -1 and removal percentage of LH and Pb 2+ in real wastewater was above 90% and 70% which indicated the great application potential.
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ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Xiangchen Kong,Chao Liu,Ming Lei,Feng Gong,Yue Han,Yuyang Fan,Ming Li,Rui Xiao
The fundamental understanding of the catalytic performance of copper-based catalysts for lignin hydroconversion is delayed compared with the empirical optimization of the catalyst preparation. Herein, we investigate the interplay between the lignin-abundant oxygen-containing functional groups and Cu active species via the catalytic β-O-4 lignin linkage hydrogenolysis. Catalyst performance data and elemental spectra characterizing the catalyst demonstrate the dominance of Cu0 in the catalysis. Remarkably, Cα–OH and Cα═O in the aliphatic chain play critical roles in this process, without which the linkage cannot be broken. These groups markedly accelerate the linkage cleavage by decreasing both the chemisorption energy between Cβ–O and Cu0 and the bond dissociation energy of the linkage. On the contrary, the methoxyl groups attached to the aromatic rings hinder the bond cleavage as a result of the steric effect. Such hindrance is significantly affected by the amount and position of the methoxyl groups. The results of this work highlight the importance of the unique structures of lignin in its reductive depolymerization catalyzed by copper-based catalysts, which appear to offer an opportunity for tailoring efficient copper-based catalysts for lignin hydrogenolysis.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Lingli Zhu,Dekui Shen,Qian Liu,Chunfei Wu,Sai Gu
Biomass transformation into high-value carbon nanomaterials plays a dual role of easing the energy material crisis and reasonable disposal of waste. Here, we employed biomass lignin as carbon source to synthesize fluorescent carbon quantum dots (CQDs) through a facile two-step method. The preparation condition is optimized at 0.3 g of acid additive and 200 ℃, 16 h of hydrothermal treatment. The resultant CQDs with the average diameter of 4.86 nm and high quantum yield of 23.68% are composed of carbon cores and surface functional groups, exhibiting the maximum green emission wavelength of 476 nm. The formation mechanism involves acid dissociation of lignin in the first step, and then the aromatic refusion of lignin fragments. The CQDs show great advantages as fluorescent nanoprobe for metal ion detection, which present an apparent and selective fluorescence quenching effect on Fe 3+ . This CQD nanoprobe has a highly sensitive response to Fe 3+ ions in the concentration of 0 ~ 300 μM with detection limit of 0.77 μM. The utilization of renewable biomass lignin in this study not only opens the avenue of the sustainable, cost-effective and mass production of CQDs, but also provides a novel alternative nanoprobe for sensing field.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2021
·
IF 5.279
Fei Li,Honglu Zhao,Ruijian Shao,Xiaoyu Zhang,Hongbo Yu
The Fenton reaction is considered to be of great significance in the initial attack of lignocellulose in wood-decaying fungi. Quinone redox cycling is the main way to induce the Fenton reaction in fungi. We show that lytic polysaccharide monooxygenases (LPMOs), through LPMO-catalyzed oxidation of hydroquinone, can efficiently cooperate with glucose dehydrogenase (GDH) to achieve quinone redox cycling. The LPMO/GDH system can enhance Fe3+-reducing activity, H2O2 production, and hydroxyl radical generation, resulting in a fueled Fenton reaction. The system-generated hydroxyl radicals exhibited a strong capacity to decolorize different synthetic dyes and degrade lignin. Our results reveal a potentially critical connection between LPMOs and the Fenton reaction, suggesting that LPMOs could be involved in xenobiotic compound and lignin degradation in fungi. This new role of LPMOs may be exploited for application in biorefineries.
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ENERGY
·
2021
·
IF 7.147
Chao Li,Yifan Sun,Dehua Dong,Guanggang Gao,Shu Zhang,Yi Wang,Jun Xiang,Song Hu,Gholizadeh Mortaza,Xun Hu
The major compounds of cellulose and lignin in biomass could have varied contributions on distribution and properties of pyrolysis products by generating the volatiles of different structures via pyrolysis. In this paper, the co-pyrolysis of cellulose or lignin with sawdust were investigated, aiming to probe the impacts of volatiles from lignin or cellulose pyrolysis on evolution of products. The results indicated that the interactions between volatiles from cellulose or lignin with that of sawdust did exist. The co-pyrolysis of sawdust with cellulose tended to promote the bio-oil production, while the co-pyrolysis with lignin enhanced the formation of biochar. The cross-polymerization of light species (i.e. radicals) from cellulose pyrolysis with heavier ones from lignin pyrolysis transformed the precursors of gases into condensable liquid, bio-oil. In comparison, the interaction of heavy species between lignin and those from sawdust produced more carbonaceous solid, biochar. Additionally, the biochar from co-pyrolysis of sawdust with cellulose possessed more oxygen-containing functionalities (i.e. C O), higher oxygen content, while lower thermal stability, while that from co-pyrolysis with lignin was opposite. The in situ Diffuse Reflection Infrared Fourier Transform Spectra (DRIFTS) analysis suggested that the volatiles from cellulose reacted with that from sawdust formed more aliphatic structures.
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