FUEL
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2021
·
IF 6.609
Zhi Yang,Bowen Luo,Riyang Shu,Zhipeng Tian,Yu Kang,Ying Chen
An effective binary catalyst by using tungstic acid (H 2 WO 4 ) and Ru/C was employed for the hydrodeoxygenation (HDO) of phenolic compounds and raw lignin-oil. H 2 WO 4 was presented as solid at ambient temperature, but it dissolved at high temperature above 100 °C and therefore functioned as an active homogeneous catalyst. This phenomenon resulted in a temperature-controlled phase-transfer behavior in the HDO of phenolic compounds. An efficient HDO performance and an exceptional reusability for guaiacol HDO were presented by this bifunctional catalyst, which can be reused more than 10 times with guaiacol conversion and cyclohexane selectivity over 90%. The comparison of traditional liquid organic and mineral acids, as well as solid acids, with H 2 WO 4 confirmed the outstanding catalytic performance of H 2 WO 4 and highlighted the advantages of H 2 WO 4 as a homogeneous catalyst. Besides guaiacol, other phenolic compounds including various monomers and dimers all exhibited good HDO results, with 100% conversion and cycloalkanes selectivity. Moreover, the raw lignin-oil can be efficiently deoxygenated under the catalysis of this bifunctional catalyst. 99.3% content of hydrocarbons was obtained in the upgraded lignin-oil, which was promising to be used as fuel directly. This catalytic system has great potential for the industrial application of lignin-oil upgrade.
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高影响因子
GREEN CHEMISTRY
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2021
·Vol. 23
·期 5
·2079-2094
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IF 10.182
Lanfang Cao,Lu Lin,Haiyan Sui,Heng Wang,Zhichao Zhang,Nianzhi Jiao,Jizhong Zhou
Microbial-driven lignin conversion has a significant impact on the biogeochemistry of global ecosystems and biomass utilization. During this process, secretion of extracellular ligninolytic enzymes is the first, essential step, yet there is a significant challenge to the secretion of these high-redox potential enzymes in bacteria, especially in Gram-negative bacteria. In this study, genome and proteome analyses enabled us to bio-design two types of extracellular secretory apparatus, both of which effectively secreted a heterologous laccase in Pseudomonas putida, up to ∼300 U mL−1. Importantly, a strong cooperation between P. putida A514 cells and the extracellular laccase, which was either released to the medium or displayed on the cell surface, was observed to significantly promote cell growth (9 × 1010 CFUs mL−1) and lignin consumption (12.5%). Chemical analyses of lignin further confirmed the effect on lignin utilization. Moreover, we demonstrated that a free laccase-A514 cell system exhibited greater effect on lignin utilization than that of a cell-immobilized laccase complex, which challenges the current view of bacterial polymer catabolism, and suggests the importance of secretory pathways and sufficient reaction surface for lignin biocatalysis. Our study advances the knowledge of secretion mechanisms in Gram-negative bacteria and provides novel insights into the lignin utilization by extracellular lignolytic enzyme-bacterial cell systems.
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ENERGY & FUELS
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2020
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IF 3.421
Xiangchen Kong,Chao Liu,Yue Han,Ming Lei,Yuyang Fan,Ming Li,Rui Xiao
The development of an economic and sustainable catalytic system was crucial for lignin-based biorefinery. Herein, we reported a low-cost Cu/CuMgAlOx catalyst with promising activity toward lignin hydrodeoxygenation (HDO) through a H2-free method. Supercritical methanol was used as the hydrogen donor, solvent, and reactant simultaneously. Guaiacol was employed as a representative lignin model compound to reveal the HDO mechanism of lignin derivatives. HDOs of guaiacol performed at 250, 275, 300, and 350 °C with durations ranging from 15 to 120 min indicated a high HDO efficiency of the catalytic system. The obtained liquid products were categorized to oxygen-containing unsaturated products (OUPs), oxygen-containing saturated products (OSPs), and cycloalkanes. A kinetic model based on a simplified reaction process containing the three following conversion steps was established: guaiacol transformed to OUPs through the initial HDO, then hydrogenated to OSPs (medium HDO), and eventually turned to cycloalkanes by the deep HDO. The deep HDO was the rate-determining step, and the apparent activation energies of the three steps were all lower than those in the literature. Phenol, 1,2-cyclohexanediol, anisole, and veratrole were the major intermediates, the HDOs of which were programed for pathway verification. Remarkably, catechol (the culprit of condensation) was not produced in this system. Overall, a detailed reaction network of guaiacol HDO was established, and the veil of Cu/CuMgAlOx-catalyzed lignin-derivatives HDO in supercritical methanol was revealed. This work paved the way for the application of Cu/CuMgAlOx catalyst in lignin-derivatives upgrading.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
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IF 5.541
Chao Li,Jun-ichiro Hayashi,Yifan Sun,Lijun Zhang,Shu Zhang,Shuang Wang,Xun Hu
Understanding evolution of the functionalities of biochar versus temperature is a prerequisite for exploring application of biochar as functional carbon materials. In this study, pyrolysis of lignin with different heating rates was conducted. The results indicated that the higher heating rate promoted formation of more gases via the accelerated cracking of both the organic components of biochar and the volatile products. In addition, the deoxygenation reactions were suppressed at higher heating rate with short residence time, leading to the biochar with lower heating value and energy yield. The in situ Diffuse Reflection Infrared Fourier Transform Spectra (DRIFTS) characterization of the lignin pyrolysis indicated monotonous increase of the abundance of =C−H, C=C and C−O−C functionalities versus increasing pyrolysis temperature. However, the −OH, −CH 3 and C−H 2 in alkanes and the C=O were not thermally stable. Abundance of −OH maintained a plateau in 200−450 °C, while that for −CH 3 and C−H 2 in alkanes also reached maximum at ca. 450 °C and the further increasing heating temperature led to significant decomposition. The decomposition of C=O started at the lower temperatures of 200–325 °C, and the lactones, unconjugated alkyl aldehydes, alkyl esters, conjugated aldehydes/ketones experienced distinct temperature-abundance histories.
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BIORESOURCE TECHNOLOGY
·
2020
·
IF 7.539
Ge Guo,Wenzhi Li,Xiaomeng Dou,Ajibola T. Ogunbiyi,Tauseef Ahmed,Baikai Zhang,Mingwei Wu
Non-noble bimetallic nanoparticles anchored on Zeolitic Imidazolate Frameworks, bifunctional ReMo@ZNB catalyst, has been demonstrated to promote Kraft lignin depolymerization. In this study, the catalytic activities under different heat treatment conditions are ranked as follows: ReMo@ZNB-700 (Air) > ReMo@ZNB-500 (Air) > ReMo@ZNB-700 (N 2 ). Particularly, bimetallic ReMo nanocatalyst with Re/Mo atomic ratio of 1/3 shows superior performance. Excellent yields of Ethyl acetate soluble products (92.18%) and Petroleum ether extracted biofuels (78%) are obtained at 300℃ and 24 h, and the calorific value is 32.33 MJ/kg. The ReMo@ZNB catalyst exhibits superior recyclability and regeneration after cycle experiment. Structural characterization results reveal that the incorporation of ReMo can engender the transformation of lattice morphology, the strength of hydrogenation and acid adsorption. The possible mechanism is based on the synergism of adsorption coupling and hydrogenation over ReMo@ZNB catalyst. The synergic action initiates potential perspectives for improving lignin hydroconversion.
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PubMed
高影响因子
BIORESOURCE TECHNOLOGY
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2020
·
IF 7.539
Simin Li,Zhongyang Luo,Wenbo Wang,Haoran Sun,Jiaqi Xie,Xiaorui Liang
Lewis-acid catalyst Nb 2 O 5 is first applied in catalytic fast pyrolysis (CFP) of enzymatic hydrolysis lignin (EHL) to produce aromatic hydrocarbons (AHs) that can be used as alternative liquid fuels. The catalyst exhibits a good talent to convert lignin into AHs with quite little polycyclic aromatic hydrocarbons (PAHs) formation. The yield of AHs reaches 11.2 wt% and monocyclic aromatic hydrocarbons (MAHs) takes up 94% under the optimized condition (Catalyst to Lignin ratio 9:1, 650 °C). No coke is generated during the reactions. The reaction sequence is proposed and verified by model compound reactions. Furthermore, DFT calculations are performed to understand the mechanisms of limitation of PAHs or char/coke formation and the efficient deoxygenation ability over catalyst. Nb 2 O 5 with Lewis acid sites is proved to be a promising catalyst for the production of AHs from lignin. This work provides a new idea on choice of catalysts for CFP of lignin in future.
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Yiqi Sun,Zhewen Ma,Xiaodong Xu,Xiaohuan Liu,Lina Liu,Guobo Huang,Lei Liu,Hao Wang,Pingan Song
It has been always attractive to design low-cost, ductile, and fully biobased polylactic acid (PLA) composites based on industrial waste lignin for promoting its practical applications in the industry. Unfortunately, existing material strategies often lead to poor processability and low ductility because of weak interfaces between lignin and PLA. Herein, we report a fully biobased functionalized lignin (Lig-g-P(LMA-co-THFMA, or Mlignin) by chemically grafting two bioderived monomers, lauryl methacrylate (LMA), and tetrahydrofurfuryl methacrylate (THFMA) via free-radical polymerization. Mlignin exhibits moderately lower melt viscosity and improved formability with PLA as compared with pristine lignin due to better interfacial combability. Because of improved interfacial adhesion, Mlignin is capable of uniformly dispersing within the PLA matrix in a submicron phase size, leading to a “sea-island” structure. As a result, the addition of 20 wt % Mlignin increases the ductility by 16 folds (from 12 to 204%) and the toughness by ∼11 folds from 4.4 to 54.6 MJ m–3 relative to the PLA matrix. Meanwhile, the PLA/20% Mlignin composite retains a tensile strength of 40.9 MPa. Such largely enhanced ductility and toughness of PLA is mainly attributed to the deformation of Mlignin that can dissipate the fracture energy during the tension process. This work not only offers a simple route to converting industrial waste lignin into value-added biobased fillers for polymers and but also provides a new approach for developing low-cost, ductile, and fully sustainable PLA to further its industrial applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Xiaomeng Dou,Xiao Jiang,Wenzhi Li,Chaofeng Zhu,Qingchuan Liu,Qiang Lu,Xusheng Zheng,Hou-min Chang,Hasan Jameel
Kraft lignin depolymerization to liquid fuels with high yields is crucial to the comprehensive achievement of sustainable and economic feasibility. Herein, we prepared a bimetallic Co-Zn/Off-Al H-beta catalyst through a two-step post synthesis method composed of dealumination and metal incorporation. The bifunctional Co-Zn/Off-Al H-beta catalyst efficiently converted Kraft lignin to liquid fuels, which was attributable to the synergistic effect of Co hydrogen binding sites and Zn Lewis acid sites on H-beta support. Catalytic hydrogenation with Co:Zn = 1:3/Off-Al H-beta catalyst at 320 °C for 24 h gave the highest yield of petroleum ether soluble product (81%, mainly monomers and dimers). Under these conditions, the liquefied lignin gave a higher heating value of 33.3 MJ/kg, which is a significant increase from 26.0 MJ/kg of Kraft lignin. The catalyst stability test showed excellent recyclability. This work provides a paradigm of improving lignin depolymerization efficiency via the combined use of Lewis acid and hydrogenation catalyst.
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高影响因子
TRANSITION METAL CHEMISTRY
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2019
·Vol. 45
·期 2
·111-119
·
IF 1.016
Song Kunpeng,Tang Cheng,Zou Zhijuan,Wu Yundang
The conversion of carbon dioxide into useful chemical raw materials is a necessary development for advancing carbon dioxide capture and storage technology. In this work, a Friedel–Crafts reaction of lignin and metalloporphyrin was used to produce a lignin-based porous organic polymer (P-(L-FeTPP)) with a surface area of up to 1153 m 2 g −1 . P-(L-FeTPP)) efficiently catalyzed the cycloaddition reactions of epoxides and CO 2 under solvent-free conditions, with porphyrin iron acting as an active center. The product yield reached up to 99.6% after 12 h under 1 MPa CO 2 and 70 °C. A turnover number of 1481 was achieved, indicating that this catalyst is much more active than its homogeneous counterpart and is one of the most efficient lignin-supported heterogeneous catalysts ever reported. This method for the in situ incorporation of a metalloporphyrin into a lignin skeleton greatly improved the stability of the metal catalyst, and P-(L-FeTPP) was readily recycled and reused more than six times without any significant loss of catalytic activity. Thus, this catalyst design is promising for practical applications, including the industrial production of cyclic carbonates.
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高影响因子
CHEMICAL PHYSICS LETTERS
·
2019
·
IF 1.901
Shuai Wang,Liqin Zhang,Guobao Sima,Ying Cui,Linhuo Gan
The lignin-derived ordered mesoporous carbon solid acid (LDMC-SO 3 H) was prepared by evaporation induced self-assembly and sulfonation using Masson pine alkali lignin as carbon source. And LDMC-SO 3 H was used as catalyst in the hydrolysis of bagasse cellulose (BSC) with crystallinity index of 70.3% pretreated using deep eutectic solvent. A glucose yield of 42.5% was obtained under the optimized conditions of reaction temperature and time of 180 °C and 7 h, initial BSC concentration of 5 mg/mL and catalyst load of 3 mg/mg. In addition, glucose yield decreased to 31.0% after five runs of LDMC-SO 3 H due to the loss of -SO 3 H groups.
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高影响因子
CELLULOSE
·
2019
·Vol. 26
·期 3
·1577-1593
·
IF 3.917
Jiang Yan,Liu Xiuyu,Yang Qiang,Song Xueping,Qin Chengrong,Wang Shuangfei,Li Kecheng
Abstract This study investigated effects of residual lignin on composition, structure and properties of cellulose fibrils and cellulose fibril-based films by comparing two groups of cellulose fibrils which contained different amounts of lignin (15% and 2%, respectively) but were similar in cellulose to hemicellulose ratio. The results showed that lignin affected the size and content of nanofibril in cellulose fibrils through initially delaying but ultimately facilitating the mechanical defibrillation. Due to higher thermal stability and strong UV absorption capability, lignin enhanced the thermal stability and UV blocking properties of cellulose fibril-based film. Hydrophobic lignin also improved the dewatering of cellulose fibrils and the hydrophobicity of cellulose fibril-based film. Lignin interfered with the interfibrillar hydrogen bonding and therefore increased the mesopore diameter of cellulose fibril network. Lignin acting as a cement in cellulose fibril-based film made the film with a more densely packed structure, a higher density and a smoother surface. However, lignin decreased the transparency of cellulose fibril-based film due to its chromophore groups and impaired the mechanical strength of cellulose fibril-based film through interfering with the interfibrillar hydrogen bonding. Graphical abstract
研究领域:
材料科学
·
植物学
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Journal of Environmental Sciences
·
2026
·
IF 6.5
Yunhang Zhang,Yue Pan,Haibin Li,Shou-Qing Ni,Lingshuai Kong,Jinhua Zhan
Carbon nanorods are obtained from lignin via a mechanochemical process. • Surface oxidation and subsequent H-bonding are key drivers for the rod formation. • Carbon nanorods exhibit abundant oxygen functional group. • Carbon nanorods/PMS efficiently remove pollutants and pathogenic bacteria. Lignin is an abundant biomass resource widely used as a precursor for high-quality functional carbon synthesis. However, transforming lignin into structurally controllable carbon nanorods remains a significant challenge. A mechanochemical approach was employed to synthesize uniform carbon nanorods (CNRs) with an average diameter of 52 nm and a length of 5.7 μm, featuring abundant oxygenated functional groups. The infrared spectroscopy results show that hydrogen bonds play a crucial role in nanorod formation. In peroxymonosulfate (PMS) activation, CNRs achieve 99.4 % bisphenol A removal within 18 min with a rate constant of 0.264 min −1 , while the CNRs membrane maintained over 90 % pollutant removal within 1400 min and exhibited 99 % bactericidal efficiency. Free radical quenching experiments and electrochemical experiments confirmed that the electron transfer and 1 O 2 were the main pathways in the CNRs/PMS system. Life cycle assessment indicates that the mechanochemical route exhibits lower environmental impacts compared to conventional chemical vapor deposition. This study offers a ball-milling strategy for designing uniform carbon nanorods with promising applications in environmental and energy-related technologies. Download: Download high-res image (211KB) Download: Download full-size image
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