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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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhongwei Wang,Xiangqian Chen,Yisheng Sun,Dongliang Hua,Shuangxia Yang,Laizhi Sun,Tianjin Li,Lei Chen
Designing highly active and stable catalysts for the selective cleavage of the C-O bond of lignin is important to convert it into high-valued aromatic compounds. Herein, a facile synthetic strategy was developed using melamine as a soft template to prepare a highly active catalyst consisting of highly dispersed Ni nanoparticles on defective N-doped carbon support. The results indicated that the decomposition of melamine during the pyrolysis process induced the nitrogen atoms into aromatic carbon. The introduction of N-doped carbon support acted as anchor points for the Ni nanoparticles, strengthening the metal-support interaction. Approximately 100 conversion of the representative lignin model compounds, including 2-phenylethyl phenyl ether, were converted into their aromatic monomers under mild conditions. The as-prepared catalyst was stable and reusable after five cycles with no apparent signs of deactivation. Moreover, the theoretical calculation revealed that N-doped carbon supported Ni-based catalyst possessed a lower activation energy of C-O bond than only carbon supported Ni-based catalyst for the C-O bond cleavage in hydrogenolysis of lignin and its model compounds.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Erhu Li,Xuliang Lin,Shirong Sun,Xueqing Qiu
The highly selective conversion of technical lignin to low-oxygen-content compounds is still challenging due to the presence of methoxy and ether bonds in natural lignin. Herein, tunable ternary deep eutectic solvents (DESs) containing choline chloride, oxalic acid, and another bifunctional reagent with a hydrogen-bond donor and nucleophilic function were used for the β-aryl ether bond cleavage or Cα-etherification of lignin followed by pyrolysis to improve the yield of methoxy-free lignin monomers. The relationship between the lignin structure and pyrolysis behavior was investigated by 2D-NMR, FTIR, GPC, XPS, TGA, TG-FTIR, EPR, etc. The DES pretreatment changed the pathway of lignin pyrolysis toward a higher yield of bio-oil and methoxy-free products. Compared with technical lignin, the yield of phenolic products after Cα-etherification with ethanol and ethylene glycol as nucleophilic reagents increased from 0.73 × 1011 to 4.10 × 1011 and 5.56 × 1011 area/mg, respectively. Besides, the introduction of ethanol and ethylene glycol is more conducive to the demethoxylation of pyrolysis products and the formation of methoxy-free phenols during pyrolysis. This work realizes the conversion of lignin to high-value phenolic products with low-oxygen-content compounds without adding catalysts by a pyrolysis strategy.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
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IF 5.9
Shuyang He,Feng Shu,Xianglin Liu,Ke Yan,Shijie Lei,Yupeng Liu,Mingu Zhou,Hang Yu,Junhua Zhang,Fangxia Yang
Pretreatment method is one of the key factors to improve the quality of nanocellulose (NC) production. As a green novel solvent, ternary deep eutectic solvent (TDES) plays an important role in production of lignin-containing nanocellulose (LNC), however, higher reaction temperature would limit its industrial application. Herein, a novel strategy of FeCl 3 -catalyzed TDES (F-TDES) pretreatment combined microfluidization was proposed to produce LNC from poplar ( PopulusL. ) at lower temperature (80 °C). The TDES was composed of choline chloride, lactic acid, and p -toluenesulfonic acid in a molar ratio of 2:10:1. When the optimum dose of FeCl 3 in per gram TDES system was 0.15 mmol (i.e. about 3.9% based on the weight of F-TDES), ribbon-like LNCs about 28.68 nm wide and 3.46 nm thick were obtained, which were smaller than that of lignin-free nanocellulose attained from the same preparation conditions. The LNC, lignin content 18.93%, displayed good dispersion stability in water and higher cellulose I crystallinity (57.8%) and thermal stability (T max =376 °C). Especially, the LNC exhibited more excellent emulsification performance and emulsion stability than NC, which was closely associated with its good amphiphilicity. Within the studied LNC concentration (0.1–0.4%) and oil/water mass ratio (20:80–50:50), increasing LNC concentration and/or oil/water mass ratio was beneficial for the stability of Pickering emulsions. The findings not only provide a milder route for producing LNC from lignocellulose , but also prove LNC would have promising prospects in emulsion systems.
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高影响因子
Biochar
·
2023
·Vol. 5
·期 1
·1-14
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IF 12.7
Chen Chao,Sun Kang,Huang Chen,Yang Mengmei,Fan Mengmeng,Wang Ao,Zhang Gaoyue,Li Bei,Jiang Jianchun,Xu Wei,Liu Junli
The structural reconstruction mechanism of lignin and cellulose-derived biochars during direct graphitization under ultra-high temperatures was intensively investigated. It was demonstrated that cellulose-derived char was almost composed of carbon microcrystallites, whereas lignin-derived char reserved some of its skeleton structures, and such structural difference played a vital role in the morphology of formed graphitic layers. The results illustrated that the graphitized lignin-derived sample under 2800 ℃ had graphitic degree of 89.53%, interlayer spacing of 0.3363 nm and electronic conductivity of 104.6 S cm −1 , while cellulose-derived sample had graphitic degree of 76.74%, layer distance of 0.3374 nm, and electronic conductivity of only 48.8 S cm −1 . Combined with the results of structural analysis of the chars derived from lignin and cellulose, it was inferred that the stable and aromatic ring containing skeleton structure in lignin was beneficial to the ring-enlarging reconstruction and the formation of large areas of continuous graphitic layers during graphitizing process, leading to high electronic conductivity. Meanwhile, the interwoven microcrystallites in cellulose-derived char strongly restricted the expanding of continuous lamellar graphitic areas even at such ultra-high temperature, causing the formation of turbostratic structure with numerous structural defects as well, and finally resulting in relatively lower electronic conductivity. This work is expected to provide theoretical guidance for preparing high-performance functional carbon materials from lignocellulosic biomass. Graphical Abstract
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
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IF 6
Geliang Xie,Guoqiang Zhu,Tong Lv,Yifan Kang,Yuhan Chen,Zhen Fang,Lujiang Xu
Co-valorization of biomass and multiple solid wastes is essential to environment protection and energy security. Herein, aromatic-rich biofuel was produced from lignin and waste polyoxymethylene (POM) via catalytic co-pyrolysis process. Commercial and cheap γ-Al 2 O 3 catalyst exhibited good catalytic performance. Series characterizations and bench-top pyrolysis experiments were conducted to illustrate the synergism between raw materials and the mechanism of aromatics formation. The TG analysis and thermodynamics calculation revealed that a remarkably positive synergistic effect existed between lignin and POM, which reduce the activation energies and make the reaction more conducive in terms of thermodynamics. Meanwhile, the yields of biochar and bio-oil increased considerably. Additionally, the operating conditions affected the product distributions significantly. The suitable mixing ratio of lignin to POM was around equal (5:5) with the bio-oil yield increased to 28.3 % and aromatic hydrocarbons selectivity increased to > 95 %. Moreover, POM, the precursor for alkylating reagents and hydrogen donors , could promote the deoxygenation reactions of phenolic intermediates and result into aromatic hydrocarbons. The acid sites of γ-Al 2 O 3 promoted series secondary cracking reactions (alkylation, deoxygenation), and thus improved bio-oil quality. Finally, the stability test showed that commercial γ-Al 2 O 3 catalyst was slightly deactivated after 4 cycles because of coke deposits and acid sites loss.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
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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Journal of Energy Chemistry
·
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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INDUSTRIAL CROPS AND PRODUCTS
·
2023
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IF 5.9
Zhongqiu Fan,Xingye An,Zhengbai Cheng,Haibing Cao,Junwei Li,Liqin Liu,Hongbin Liu
The main non-wood lignocellulose resource, wheat straw, has been utilized in bio-mechanical pulping process for paper industry to alleviate feedstock shortages, reduce environmental pollution, and lower carbon emissions as well. However, the wheat straw-based bio-mechanical pulping effluent (BMPE) could cause water pollution and resource waste if not properly handled. The efficient extraction of lignin biomass from BMPE is still a great challenge. The novelty of this study is to propose a facile process for efficient extraction of lignin with high yield, high purity and controllable morphology from wheat straw based BMPE via a commercialized technique, LignoForce™ process, which has been industrially applied in lignin extraction from wood based Kraft pulping black liquor. Considering the unique attributes of wheat straw (non-wood) based BMPE, we successfully improved the LignoForce™ technology for high efficient lignin extraction. The extracted lignin from BMPE was characterized for its chemical properties, ash content, monosaccharide composition, controllable morphology, particle size/distribution, and molecule weight/distribution at varying oxygen dosages and oxidation temperatures. The resultant lignin particles possess comparable regular spherical morphology with controllable particle size/ distribution. Additionally, the yield and ash content of the lignin extracted from BMPE and chemical-mechanical pulping effluent (CMPE) of wheat straw were compared and analyzed to evaluate the feasibility of the improved LignoForce™ technology utilized in non-wood BMPE with high extraction efficiency. The study found that the practical successive LignoForce™ treatments, including oxidation process (O 2 ), CO 2 , and H 2 SO 4 acidification procedures, showed great potential in obtaining high-yield and high-quality acid-precipitated lignin with controllable morphology from the non-wood (wheat straw) based BMPE.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Xiaoyan Zeng,Yongfa Huang,Tingzhen Li,Zheng Lian,Ren Zou,Xinwen Peng
As a wood containing many ordered cell cavities and blood vessels, eucalyptus is an ideal precursor material in preparing hierarchical porous carbon electrodes for Zn-air batteries. However, insufficient micro-mesoporous and minor active sites inhibit the application of wood-directly derived carbon materials in Zn-air batteries. Hence, a simple and cost-effective formic acid pretreatment method was proposed to prepare nitrogen-doped bulk phase catalysts with abundant micro-mesoporous and enough high active sites from eucalyptus. Formic acid pretreatment selectively removed part of lignin and hemicelluloses , thus generating abundant nanopores and contributing to the introduction of more nitrogen active sites. Moreover, the obtained bulk carbon had high mechanical strength and wonderful electrical conductivity, containing cross-linked networks and natural ion transport channels. Benefiting from the above advantages, the bulk carbon catalyst could be directly used as self-supported cathode, and the resulting Zn-air batteries achieved a long cycle life of more than 300 h. This work provides a simple and feasible method for the development of biomass-derived hierarchical bulk-phase porous carbons for energy-related applications.
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高影响因子
BIOMASS & BIOENERGY
·
2023
·
IF 6
Jiubing Zhang,Bo Chen,Yuanyuan Ge,Zhili Li
The efficient depolymerization of lignin for the production of high-value chemicals is essential for the development of a sustainable and competitive biorefinery . In this study, we report the preparation of homologous biochar-supported inlaid Cu–Ni catalysts (Cu x Ni y /BC) using a one-step method, and their application for lignin depolymerization in mild water without the need for external hydrogen, additives, or co-catalysts. The Cu 1 Ni 3 /BC (0.05 g catalyst, 8 h, 280 °C, and 18 mL water) showed exceptional catalytic activity , with a monophenol yield of 94.35 ± 2.92 mg/g, bio-oil yield of 68.98 ± 1.42%, and a lignin conversion rate of 92.36 ± 1.99%, which outperformed both the biochar support and monometallic catalysts. The outstanding catalytic performance of Cu 1 Ni 3 /BC was attributed to its strong metal-support interaction, alloy sites, and well-dispersed nanoparticles . Reusability experiments demonstrated that the Cu 1 Ni 3 /BC exhibited relatively good stability for up to four reuses, with only a 2.32% reduction in catalytic activity per cycle. Mechanism investigation revealed that the Cu 1 Ni 3 /BC, with its abundant mesoporous structure and enhanced acid sites, displayed excellent deoxygenation ability, enabling effective cleavage of C–O/C–C bonds and the production of G-type phenols . This approach provides new insights into the large-scale utilization of lignin for the production of high-value chemicals.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
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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PubMed
高影响因子
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