INDUSTRIAL CROPS AND PRODUCTS
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2023
·
IF 5.9
Xiaohui Yang,Chengjun Tang,Lihong Hu,Yonghong Zhou,Minghao Zhou
The industrial production of monophenols was mainly dependent on fossil resources, due to growing energy demand and escalating environmental issues, more efficient and sustainable strategy, such as utilization of biomass as raw materials to economically produce monophenols, was desired, which could liberate us from the reliance on fossil resource and was of great industrial and social significance. Herein, a novel strategy was reported to produce biomass-derived monophenols from lignin by directly deconstructing C-O bond under mild conditions. A series of NiM-MOFs (M=Co, Mo, and Cu) derived bimetallic catalysts were synthesized via a simple hydrothermal method, which were characterized by XRD , SEM , TEM , XPS and NH 3 -TPD. The synergistic effect between the Ni and Mo greatly improved the catalytic activity and inhibited the transformation to by-products. In addition, we explored a new binary solvents system of MeOH-THF to effectively enhance the selectivity of monophenols. Under optimal catalytic conditions, Ni4Mo1/C-BN catalyst could break the C-O bonds in lignin dimer under 160 ℃ to afford phenol and benzoic acid , and the possible reaction pathway was proposed. The high yield of lignin oil from the oxidation of various realistic lignin also confirmed the superiority of this catalytic system. The lignin depolymerization products were characterized by element analysis, GPC and GC-MS, confirming the presence of mainly guaiacyl-type (G) products, while the highest yield was assigned to vanillin.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhiyi Huang,Huan Wang,Jiahao Du,Xiaochun Liu,Guoyi Pan,Xingshan Yin,Wenjing Lin,Xiaofeng Lin,Yingjuan Sun,Guobin Yi,Li Niu
The preparation of lignin-based polyurethanes with excellent mechanical properties and recyclability remains extremely challenging because of the poor compatibility of lignin and matrix. Inspired by the multiple structures of spider silk and pearl layers, high-strength, heat-resistant and recyclable lignin-based polyurethanes (LPUs) were prepared by introducing weak hydrogen bonds, strong hydrogen bonds and dynamic silyl ether covalent bonds. Multiple hydrogen bonds provided a large energy dissipation mechanism. The covalent linkage between lignin and matrix promoted their compatibility and formed a robust cross-linking network. Depending on the multi-level dynamic interactions, the prepared elastomer exhibited a mechanical strength of 73 MPa, which was 1.9 times higher than that of the blank sample, with an initial thermal decomposition temperature of 310.5 °C and a good recyclability. Especially, the mechanical strength of LPUs was up to 99 MPa after mechanical training. In addition, the abundant conjugated structure of lignin endowed LPUs with an excellent photothermal conversion ability. Under the irradiation of NIR light with 4000 w m −2 , the surface temperature increased to 95 °C within two minutes, exhibiting a stable photothermal performance even after 6 cycles. This work showed the application prospects of LPUs in the fields of high strength engineering materials and photo-induced actuators.
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CHEMOSPHERE
·
2023
·
IF 8.8
Suwan Cui,Bohao Qi,Hao Liu,Xiaojun Sun,Rui He,Junshuai Lian,Yiming Li,Jinren Lu,Mutai Bao
Rapid and efficient recovery of oil spill is the key link for oil spill remediation, and also a great challenge. Here, the organogelator-polymerized porous matrix composed of adsorbents and organogelators can provide a new strategy for solving this problem. The gelling mechanism of aluminum 12-hydroxystearate (Al HSA) to form spherical nano micelles in solvents was investigated via UV–vis, FT-IR, and XRD . A creative method for aluminum soap-lignin gelator (OTS-AL/Al HSA) syntheses was put forward through the saponification of 12-hydroxystearic acid (HSA) and lignin via epichlorohydrin (ECH) crosslinking. By adjusting the ECH content, the growth of Al HSA nanoparticles (15–40 nm) on lignin can be realized, and the accordingly increased roughness endowed gelator with better hydrophobicity (WCA of 134.6°) before octadecyltrichlorosilane (OTS) modification. Thanks to the porous structures, the gelator powder exhibited a high sorption capacity in the range of 3.5–5.2 g g −1 for oils and organic solvents. Rheological studies demonstrated high mechanical strength of gels (>1.6 × 10 5 pa) and the gelator still retained 70% sorption capacity after 6 gelation-distillation cycles. The gelation characteristics of OTS-AL/Al HSA were attributed to the rapid sorption of oils by lignin and the self-assembly of Al HSA nano micelles on lignin to form an aggregated network structure trapping oils, thus realizing the synergistic effect of oil sorption-gelation.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2023
·
IF 11.4
Ying Xu,Cheng-Ye Ma,Shao-Chao Sun,Chen Zhang,Jia-Long Wen,Tong-Qi Yuan
In this study, light-colored lignin was extracted from bamboo shoot shells (BSS) using a hydrated deep eutectic solvent (DES) pretreatment. The hydrated DES used in pretreatment consist of formic acid, benzyl triethylammonium chloride (BTEAC) and water. The pretreatment using a hydrated DES containing 30% water (H30) demonstrate efficient delignification (82.9%). Additionally, the hydrated DES protected the β- O -4 linkage from excessive cleavage and recondensation as well as keep the light-colored of lignin. Moreover, the hydrated DES extracted lignin exhibits superior antioxidant performance and tyrosinase inhibitory capacity compared to the control. Notably, incorporating 5% lignin of H30-extracted lignin into a commercial suncream led to a remarkable enhancement of the SPF value, elevating from 14.8 to 32.6. In summary, the proposed hydrated DES pretreatment method offers significant benefits for extracting light-colored lignin, thereby promoting the multifunctional application of lignin in cosmetics.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
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IF 8.2
Dan Meng,Hailiang Wang,Yuchun Li,Jian Liu,Jun Sun,Xiaoyu Gu,Haiqiao Wang,Sheng Zhang
A multifunctional lignin derivative nanoparticle (C-P-Lignin) was synthesized by grafting phenyl dichloro sphosphineoxid and 1, 4-dimethoxyacetylene stepwise on the lignin, then it was applied to prepare the thermoplastic polyurethane (TPU) composite with improved mechanical properties, oxidation resistance, and flame retardancy. The tensile strength , the elongation at break, and the toughness of the TPU/2C-P-Lignin sample reached 28.3 MPa, 941 %, and 139.0 MJ/m 2 respectively, which were increased by 39.0 %, 3.4 %, and 33.9 % respectively compared with that of the control TPU sample. The anti-fatigue property was also improved. More importantly, the mechanism of the improved mechanical properties was also calculated and simulated by FTIR and Materials Studio software. The TPU/2C-P-Lignin sample exhibited superior oxidation resistance during the process of photoaging and thermal oxidative aging. Furthermore, the peak heat release rate and the smoke production rate for theTPU/2C-P-Lignin sample was reduced by 50.0 % and 53.8 % compared with that of the control TPU. The reason was that the C-P-Lignin is conducive to the formation of uniformly distributed carbon layers. It is expected that this work can provide a new method for expanding the utilization of waste wood as a multifunctional lignin-based filler to improve fire safety and extend the service life of TPU polymers.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Jianglin Liu,Linjun Wu,Dalang Chen,Quanzhou Xu,Liheng Chen,Xuliang Lin,Yanlin Qin
The electrocatalytic hydrogen production technology using green energy can reduce the dependence on traditional fossil fuels and the net emission of carbon dioxide. However, the high overpotential and low efficiency of the oxygen evolution reaction (OER) on the anode limit the overall water splitting. Here, carboxylic acid ligands with coordination function were designed and synthesized by modifying the surface functional groups of lignin. Bimetallic functionally-doped lignin-derived carbon materials (Fe 4 Ni 4 @NC) were synthesized by continuous ion layer adsorption and pyrolysis process using Fe and Ni transition metals as source and template. The catalyst requires only 214 mV of overpotential to produce 10 mA·cm −2 , which has much faster catalytic kinetics. Theoretical calculation shows that the energy barrier of rate-determining step in OER is reduced by appropriate feed ratio and nano-size. The facile strategy opens up an economical and efficient solution for designing OER electrocatalysts with high catalytic activity and excellent stability.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Hanbyeol Kim,Jinho Lee,Yoonsoo Kim,Jeong-Myeong Ha,Young-Kwon Park,Dionisios G. Vlachos,Young-Woong Suh,Jungho Jae
Although there are many studies on the noble metal-based catalysts for the hydrodeoxygenation (HDO) of lignin model compounds such as phenols, HDO studies on lignin biomass pyrolysis oil are relatively scarce. Owing to its complex composition (i.e., a mixture of phenolic monomers and oligomers), the activity and stability of the catalysts for the HDO of pyrolysis oil are significantly different from those for the model compounds. In this study, the catalytic performances of typical HDO catalysts, that is, Ru, Pd, Ru-Re supported on carbon, and the effects of process parameters such as solvent, temperature, and space velocity were investigated for the real lignin pyrolysis oils in a continuous-flow trickle bed reactor system for the first time. We demonstrated that proper tuning of catalyst composition and process parameters allows for producing the deoxygenated hydrocarbon mixtures which can be used for gasoline, jet fuel, and diesel fuels. Specifically, activated carbon promoted the HDO of lignin oil more effectively than acidic supports like HZSM-5 and TiO 2 due to the weak adsorption of phenolic molecules. Among the different metals, Ru-Re supported on carbon exhibited the highest deoxygenation activity due to the synergy of the two metals. Tetrahydrofuran was the best solvent for lignin oil processing due to its high solubility and inertness to other side reactions (e.g., excess alkylation with ethanol solvent). The use of low space velocity of 0.2 h −1 and intermediate temperature of 350 °C resulted in the highest yield of the upgrade oil (∼25 wt%) simultaneously with the high level of deoxygenation (O/C < 0.04), mainly consisting of branched cycloalkanes. The causes of the catalyst deactivation and regeneration process are also discussed to provide practical significance.
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ChemSusChem
·
2023
·Vol. 16
·期 17
·e202300357
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IF 8.4
Yinan Tang,Lu Lu,Xiaoxian Zang,Buhuan Wang,Xiangrong Ye
Graphical Cellulose and lignin blend as carbonaceous precursor paves a feasible way to break through the restriction by intrinsic proportion of cellulose and lignin in natural biomass, allowing for tailoring and optimizing composition, structure and porosity of resultant activated carbon (AC) materials to promote power density, energy density and rate performance of supercapacitors. KOH-activated carbon materials prepared from biomass-derived carbon source, cellulose and lignin, were compared. Mixtures of different ratios of cellulose and lignin were used to partially mimic biomass as carbon source. This allows tailoring and optimizing of the KOH activated carbon materials by getting rid of the restriction of the intrinsic proportion of cellulose and lignin in specific biomass. The results indicate that cellulose use results in a more porous structure, whereas lignin use leads to more partially activated graphite structure. The activated carbon material (CL1) prepared from blend of cellulose with lignin in mass ratio of 1 : 1 exhibits a high specific surface area of 2000.39 m 2 g −1 , and in TEABF 4 /ACN (tetraethylammonium tetrafluoroborate dissolved in acetonitrile) electrolyte it showed a maximum specific capacitance of 136.10 F g −1 , a maximum energy density of 18.11 Wh kg −1 , and a capacitance retention of 85.04 % under current density as high as 15 A g −1 .
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高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 11
·4469-4481
·
IF 9.8
Pengcheng Liu,Yuanlong Guo,Gu Guo,Lei Dai,Gang Hu,Haibo Xie
In this work, a series of new lignin-graft copolymers were successfully prepared through enzymatic hydrolytic lignin (EHL)-initiated ring-opening alternating copolymerization of 3,4-dihydrocoumarin (DHC) and epoxides (EPO) through organocatalysis. A series of EPOs, including styrene oxide (SO), propylene oxide (PO), cyclohexane oxide (CHO) and lignin-derived-2-(2-methoxy-4-methyl-phenoxy) (MPO), together with DHC, were selected as model compounds to prepare EHL-g-P(DHC-alt-EPO), demonstrating the tailor-made potential of this synthetic protocol. The reaction conditions were optimized and the structures and thermal properties of EHL-g-P(DHC-alt-EPO) were fully elucidated by 1H, 13C and 31P NMR, FTIR spectroscopy, MALDI-TOF MS and GPC, DSC, and TGA. It was found that EHL-g-P(DHC-alt-SO) with a monomer conversion of 81.52%, DP of 3.21 and Mn of 62.9 kDa was prepared at a molar ratio of 5 : 5 : 1, 140 °C and 24 h. The UV shielding properties, antioxidant activity and biocompatibility of the as-prepared EHL-g-P(DHC-alt-EPO) was systematically evaluated. As a ‘proof of concept’ application, the potential of EHL-g-P(DHC-alt-SO) as an active ingredient in sunscreen was demonstrated, and a high sun protection factor (SPF) of 22.42 was achieved at 5 wt% dosage of EHL-g-P(DHC-alt-SO) in the cream, and the possible mechanism for the outstanding performance is also discussed.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Zhongwei Wang,Xiangqian Chen,Xinlin Xie,Shuangxia Yang,Laizhi Sun,Tianjin Li,Lei Chen,Dongliang Hua
The utilization of lignin to produce high value-added chemicals remains a significant challenge, this study reports the synthesis of highly active nitrogen-doped carbon nanotubes to support nickel-based catalysts via a two-stage pyrolysis process using a mixture of melamine and nickel acetate. The catalyst morphology is controlled through the use of melamine, the doped pyridinic nitrogen serves as an anchoring site for Ni metal, facilitating the dispersion of Ni metal and the formed Ni-Nx bond enhanced the stability of the catalyst. Additionally, the electron transfer between Ni and N atoms promoting the activation of hydrogen on the metallic nickel surface, which together with the aforementioned factors, contributes to the cleavage of the C-O bond in lignin, with 23.1% monomer yield under mild conditions. The density functional theory (DFT) calculations reveal that doped nitrogen atoms can provide electrons to carbon atoms, resulting in an electron-rich state that facilitated the adsorption of hydrogen.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Boyu Du,Hongwei Zhu,Jingyu Xu,Yating Bai,Qingyu Wang,Xing Wang,Jinghui Zhou
Recently, multifunctional lignin-based materials are gaining more and more attention due to their great potential for low-cost and sustainability. In this work, to obtain both an excellent supercapacitor electrode and an outstanding electromagnetic wave (EMW) absorber, a series of multifunctional nitrogen-sulphur (N-S) co-doped lignin-based carbon magnetic nanoparticles (LCMNPs) had been successfully prepared through Mannich reaction at different carbonization temperature. As compared with the directly carbonized lignin carbon (LC), LCMNPs had more nano-size structure and higher specific surface area. Meanwhile, with the increase of carbonization temperature, the graphitization of the LCMNPs could also be effectively improved. Therefore, LCMNPs-800 displayed the best performance advantages. For the electric double layer capacitor (EDLC), the optimal specific capacitance of LCMNPs-800 reached 154.2 F/g, and the capacitance retention after 5000 cycles was as high as 98.14 %. When the power density was 2204.76 W/kg, the energy density achieved 33.81 Wh/kg. In addition, N-S co-doped LCMNPs also exhibited strong electromagnetic wave absorption (EMWA) ability, whose the minimum reflection loss (RL) value of LCMNPs-800 was realized −46.61 dB at 6.01 GHz with an thickness of 4.0 mm, and the effective absorption bandwidth (EAB) was up to 2.11 GHz ranging from 5.10 to 7.21 GHz, which could cover the C-band. Overall, this green and sustainable approach is a promising strategy for the preparation of high-performance multifunctional lignin-based materials.
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Molecular Catalysis
·
2023
·
IF 4.6
Haoquan Guo,Xinyu Lu,Yue Yang,Jinhe Wei,Lizhi Wu,Li Tan,Yu Tang,Xiaoli Gu
Alkyl phenol is an essential chemical intermediate that is in high demand in the chemical industry. The synthesis of alkyl phenols from lignin-derived molecules is one of the most promising routes for utilizing biomass resources. Herein, we report the catalytic hydrodeoxygenation (HDO) of dihydroeugenol (DHE) to alkyl phenols over a highly dispersed Pd/α-MoC catalyst with a substrate conversion of 98% and a selectivity of 96% to alkyl phenols. The Pd/α-MoC catalyst prepared by co-precipitation and temperature-programmed carbonization exhibits exceptional HDO activity under mild conditions with a low H 2 pressure (1–10 bars). The characterizations of the catalyst suggest that Pd are highly dispersed on the α-MoC matrix. The reaction mechanism was investigated using the substrate scope experiments. Under ambient pressure, the abundant oxygen vacancies and acidity sites on Pd/α-MoC enable the selective hydrodeoxygenation of lignin monomers.
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