CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiuwen He,Tian Bai,Jiqing Lu,Yi Hu,Qingxiang Wang,Jie Yan,Hang Yao,Guangping Han,Wanli Cheng
Biomass-based anisotropic hydrogels are severely limited in the practical production and applications due to the weak mechanical properties, time-consuming preparation process and toxic chemical reagents. Herein, a high-strength anisotropic bamboo-based hydrogel is fabricated via in situ lignin modification of natural bamboo and flexibility process, with directionally porous structure and superior mechanical properties. The lignin modification with an UV photocatalytic oxidation process maintains the heterostructure of natural bamboo and exposes polar groups, which provide the bonding sites for subsequent flexibility process. Then, the flexible polyacrylamide (PAM) molecular chains are polymerized in the modified bamboo (photonic bamboo) to construct superior-strength anisotropic bamboo/PAM composite hydrogel (BPCH). The synthesized BPCH has an axial tensile strength (123.5 MPa) and a Young's modulus (3.46 GPa) that significantly outdistance all previous biomass-based hydrogels. Benefiting from the unique porous micro-nanostructure, the BPCH serves as an excellent and stable nanofluidic channel for ion-selective transport and presents the ion conductivity of 5.75 × 10 -4 S cm −1 at a low content. Additionally, the BPCH presents stable bending sensitivity to monitor both macroscopic and tiny human actions, such as finger bending, etc. This design offers a high-strength biomass templates and green process for next-generation anisotropic hydrogels, realizing the high value utilization of the bamboo in the micro/nanofluidic and sensor fields.
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GREEN CHEMISTRY
·
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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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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MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Guobao Sima,Linhuo Gan,Longjun Chang,Ying Cui,Ranjith Kumar Kankala
Lignin can be used as a green and sustainable substitute for phenol in the preparation of ordered mesoporous carbon using phenol resin prepolymer as precursor owing to the availability of aromatic ortho -positions in the lignin structure. To further improve the reactivity towards formaldehyde and increase the substitution degree of phenol, masson pine alkali lignin (MAL) was pretreated by an acidic deep eutectic solvent (DES). It was found that adding an appropriate amount of water to DES showed beneficial attributions to the reduction in pretreatment time and the upsurge in the phenolic hydroxyl content of regenerated lignin (DAL). The content of β - O -4 ether bond in MAL was almost cleaved. More importantly, the contents of syringyl and guaiacyl units were decreased. In contrast, the content of p -hydroxyphenyl (H) units was increased obviously, thereby facilitating lignin to react with formaldehyde. Results showed that the optimized DAL with higher content of H units was an appropriate candidate for substituting 100% of phenol in the preparation of highly-ordered lignin-derived mesoporous carbon (LDMC). Finally, the optimized LDMC exhibited high specific capacitance of 197.32 F g -1 at current density of 0.2 A g -1 , high capacitance retention of 84% at current density of 20 A g -1 , superior cyclic stability with capacitance retention rate of 99.09% after 10000 cycles and high energy density of 6.85 Wh∙kg −1 at power density of 100 W kg −1 .
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
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IF 6.953
Xinxiang Li,Mengfan Yang,Wan Zhang,Kunlin Chen,Chaoxia Wang
A durable and reversible acid-induced discoloration azobenzene UV-curable lignin-based waterborne polyurethane polymeric dye (EDA-ULPD) is prepared from lignin, azobenzene and pentaerythritol triacrylate(PETA) by chemical modification of waterborne polyurethane. Lignin and PETA are chemically bonded to the polyurethane chain to improve thermal stability , UV resistance and color fastness, while also endow the polymeric dye with UV curing performance, which is a green and environmentally friendly fixing way. The acid-induced discoloration property of EDA-ULPD with azobenzene chromophore side chain is comparable to those of 4-ethyl-4-2,2′-dihydroxy diethylamine azobenzene (EDA). As the pH value decreases from 7 to 1, the maximum absorption peak of EDA-ULPD from 420 nm to 530 nm, and the color change from yellow to pink due to the transformation of EDA molecular structure from diazo to hydrazone. Interestingly, when EDA-ULPD is fixed to the fabric in the way of UV curing, its printed fabric exhibits the performance of high concentration acid-induced discoloration (1 mol·L −1 HCl) due to the cross-linked structure formed by EDA-ULPD. The acid-induced discoloration property of EDA-ULPD printed fabrics also presents outstanding repetitious stability. The stimulus response printed fabric with reversible high concentration acid discoloration possesses a broad application prospect in smart textiles.
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Biofuels Bioproducts & Biorefining-Biofpr
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2021
·Vol. 15
·期 4
·1110-1125
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IF 4.102
Tian He,Wenxiang Zhu,Mingyou Liu,Xiaofei Tian,Fangeng Chen
Highly reactive polyols were prepared from modified acetic acid lignin (AAL) by a two-step combination of mild hydrothermal degradation and hydroxylation. The AAL-based polyols became relatively reactive and compatible with diisocyanate, with a reduction in the number average molecular weight (M n ) from 2923 to 684 g/mol and an increase in the hydroxyl content from 5.21 to 9.13 mmol/g. The mechanical performance and thermal properties of the AAL-based polyurethane elastomers (LPUEs) strongly depended on the molecular weight and hydroxyl content of the AAL-based polyols in the partial substitution of polytetramethylethylene ether glycol (PTMEG). This study proposed the prospective utilization of AAL as an alternative resource in the synthesis of polymers and biomaterials. © 2021 Society of Industrial Chemistry and John Wiley & Sons Ltd.
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INDUSTRIAL CROPS AND PRODUCTS
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2021
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IF 5.645
Wei Liu,Chenxi Ning,Ranran Sang,Qingxi Hou,Yonghao Ni
Value- added utilization of carbon-rich lignin has become an urgent and attractive research topic due to its abundance, low cost, and sustainability. How to convert lignin in an efficient and green strategy is the bottleneck limiting its valorization. Herein, a phosphorous acid (P) assisted hydrothermal process to produce lignin-derived graphene quantum dots (P-LGQDs) was developed. The as-prepared P-LGQDs was comprehensively characterized, and explored in photocatalysis. The P-LGQDs have a narrow particle size distribution, excellent electronic and optical properties, and a good pH-responsiveness. The P-LGQDs was further used to construct P-LGQDs/g-C 3 N 4 heterojunction, showing excellent photocatalytic degradation ability towards methylene blue and model lignin (94.6 % and 93.1 %, respectively). This present study offers a universal strategy for the value-added utilization and valorization of lignin.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Xiangcheng Shan,Yumeng Zhao,Shufeng Bo,Liyu Yang,Zuoyi Xiao,Qingda An,Shangru Zhai
Phosphorus (P) has brought a series of environmental problems while benefiting mankind. To reclaim phosphorus from wastewater efficiently and conveniently, a novel magnetic adsorbent with aminated lignin/CeO 2 /Fe 3 O 4 composites (AL-NH 2 @Fe 3 O 4 -Ce) possessing a high affinity to phosphate and easily separated from aqueous solutions was developed in this work. The characterization results revealed that Fe and Ce elements have been doped into the aminated lignin successfully. Batch experiment results convinced that the maximum phosphate adsorption capacity of AL-NH 2 @Fe 3 O 4 -Ce was 183.72 mg P/g at pH = 3, which was roughly 4.5 times greater than aminated lignin and 8.5 times greater than cerium oxide, respectively. The adsorption isotherm was fitted well by the Langmuir model, and the adsorption kinetics was in line with the pseudo-second-order model. The adsorption thermodynamics indicated the adsorption process was spontaneous and naturally exothermic. Additionally, AL-NH 2 @Fe 3 O 4 -Ce exhibited high selectivity towards phosphate over common coexisting anions (Cl − , NO 3 − , HCO 3 − , SO 4 2− and F − ). After five consecutive cycles, the adsorption performance of AL-NH 2 @Fe 3 O 4 -Ce decreased by only 16% compared with the fresh adsorbent, indicating that AL-NH 2 @Fe 3 O 4 -Ce exhibited excellent recycling ability. The results of XPS analysis and batch experiments showed that the possible mechanisms were electrostatic attraction and inner-sphere complexation. The tailored interfacial chemistry affinity to phosphate as well as endowed magnetic property reveled AL-NH 2 @Fe 3 O 4 -Ce could be adopted as an up and coming adsorbent in phosphate removal process.
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高影响因子
FUEL
·
2021
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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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ENERGY & FUELS
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2020
·
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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BIORESOURCE TECHNOLOGY
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2020
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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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高影响因子
BIORESOURCE TECHNOLOGY
·
2020
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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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