Biomass Conversion and Biorefinery
·
2022
·
IF 4.05
Zhang Yameng,Shen Xinming,Hu Lei,Wu Zhen,Wang Xiaoyu,Jiang Yetao
The Meerwein-Ponndorf-Verley (MPV) reduction is an extremely attractive strategy for the selective hydrogenation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) in which constructing a low-cost and high-efficiency catalyst is very essential and crucial. In this work, the enzymatic hydrolysis lignin (EL), which is a waste residue in the production process of lignocellulosic ethanol, was firstly and directly adopted as the cheap organic ligand to prepare a new zirconium-lignin hybrid catalyst (Zr-EL) by a simple solvothermal self-assembly method. Amazingly, Zr-EL displayed superior catalytic activity for the MPV reduction of HMF to BHMF, providing 98.9% yield with a high turnover frequency (TOF) of 10.86 h -1 in 2-propanol ( i PrOH) at 140 °C for 4 h. Intensive characterization and analysis results indicated that this superior catalytic activity of Zr-EL was principally attributed to the cooperative effects of Lewis acid-base sites (Zr 4+ -O 2− ) under the assistance of good hydrophilicity. Additionally, Zr-EL showed excellent catalytic stability, and when it was recovered and reused for five successive reaction cycles, an apparent loss in the yield of BHMF was not observed. More meaningfully, Zr-EL also exhibited outstanding applicability, allowing it to convert various ketone and aldehyde compounds to the corresponding alcohol products with satisfactory yields in i PrOH via MPV reduction. Conclusively, this work presents a newfangled idea to utilize the low-rank biorefinery residues and construct more practical zirconium-based catalysts for the selective synthesis of high-value chemicals. Graphical abstract
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2022
·Vol. 24
·期 4
·1570-1577
·
IF 11.034
Ruixue Yangcheng,Jiansu Ran,Zhaohui Liu,Yuntong Cui,Jianjian Wang
Efficient production of high value-added chemicals and biofuels via low-temperature chemoselective HDO of lignin derivatives in water is still a challenge. Here, we construct a low-cost, active and stable Pd/PCE catalyst using phosphoric acid-modified commercial Celite (PCE) as the support, and this catalyst exhibits excellent activity in low-temperature HDO of vanillin as well as other lignin derivatives in water. The superior catalytic performance is due to the presence of P species on the surface of Pd/PCE, accelerating the selective conversion of the intermediate into the final product. Detailed experimental and mechanistic studies reveal that the rapid conversion of the intermediate to the final product proceeds via a free-radical process in an interfacial microenvironment created by intimate interacting between the P species and Pd NPs. The insights of this work provide a new low-cost catalytic system for efficient production of valuable chemicals and future biofuels from lignin derivatives.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Baikai Zhang,Wenzhi Li,Xu Li
This work is dedicated to the selective conversion of lignin. A nickel, tin, and sulfur-doped aluminum phosphate zeolite catalyst was developed for the selective production of lignin-derived monomers. The acidity and hydrogenation sites of this catalyst can be flexibly adjusted, and it exhibits a high yield (26.7%) for monomers with a nearly 68.8% conversion of lignin at 235 °C. The results show that Brønsted acid can increase the conversion of lignin and has a high selectivity for trans-ferulic acid, while Lewis acid and hydrogenation sites can promote the production of monomers with low oxygen content. The excellent stability and simple preparation method provide the possibility for the application of this depolymerization technology. This work could be a reference for the development of lignocellulosic biomass.
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Jiajun Yu,Bingbing Luo,Yihan Wang,Siyu Wang,Kai Wu,Chao Liu,Sheng Chu,Huiyan Zhang
In this study, a simple and rapid method was proposed to synthesize orthorhombic α-Mo 2 C as catalyst for lignin catalytic pyrolysis. Biomass in-situ pyrolysis products were used as the carbon source and supporter, the carbonization of Mo precursor was realized under rapid heating. Experimental results show that Pine-Mo 2 C catalyst can achieve lignin pyrolysis vapor bond breaking and deoxidation under normal pressure, and the yield of monocyclic aromatic hydrocarbons is 13.26 wt%, of which aromatic hydrocarbons with side chain account for 74%. The side chain aliphatic hydrocarbons of lignin are effectively retained, and hydrogen consumption is minimized. The characterization of catalyst and experiments of guaiacol, 2-phenoxy-1-phenylethanol and 4,4′-biphenol shows that efficient deoxidation is due to targeted attack of catalyst on C-O. Therefore, Pine-Mo 2 C shows excellent activity in promoting direct bond breaking deoxidation of lignin.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 10
·4088
·
IF 4.6
Feng Li,Wenzhi Lv,Dena Huang,Chenglu Zeng,Runping Wang
The molecular weight of lignin extracted from lignocellulosic biomass is an important factor in determining its valorization in industrial processes. Herein, this work aims to explore the extraction of high molecular weight and bioactive lignin from water chestnut shells under mild conditions. Five kinds of deep eutectic solvents were prepared and applied to isolate lignin from water chestnut shells. The extracted lignin was further characterized with element analysis, gel permeation chromatography, and Ultraviolet-visible and Fourier-transform infrared spectroscopy. The distribution of pyrolysis products was identified and quantified with thermogravimetric analysis—Fourier-transform infrared spectroscopy and pyrolysis-gas chromatograph-mass spectrometry. The results showed that choline chloride/ethylene glycol/p-toluenesulfonic acid (1:1.8:0.2 molar ratio) exhibited the highest fractionation efficiency for lignin (84.17% yield) at 100 °C for 2 h. Simultaneously, the lignin showed high purity (90.4%), high relative molecular weight (37,077 g/mol), and excellent uniformity. Furthermore, the aromatic ring structure of lignin remained intact, consisting mainly ofp-hydroxyphenyl, syringl, and guaiacyl subunits. The lignin generated a large number of volatile organic compounds during the depolymerization process, mainly composed of ketones, phenols, syringols, guaiacols, esters, and aromatic compounds. Finally, the antioxidant activity of the lignin sample was evaluated with the 1,1-diphenyl-2-picrylhydrazyl radical scavenging assay; the lignin from water chestnut shells showed excellent antioxidant activity. These findings confirm that lignin from water chestnut shells has a broad application prospect in valuable chemicals, biofuels and bio-functional materials.Keywords:deep eutectic solvent;lignin;water chestnut shell;antioxidant activity;pyrolysis
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 34
·16043-16049
·
IF 3.3
Hongbo Yu,Fei Zhang,Shuibo Wang,Yang Cong,Shiwei Wang,Lin Zhu
Hydrodeoxygenation of lignin-derived phenolic compounds to produce alkanes is a promising method used for mitigating fossil energy consumption, but they often require high temperature and high pressure, resulting in their poor catalytic stability and durability. In this study, we encapsulated ∼3.9 nm active metal Rh nanoparticles (NPs) into ∼40 nm hollow mesoporous aluminosilicate nanospheres (HMANs) to synthesize M@Alx–mSiO2 nanoreactors with adjustable Al contents for guaiacol hydrodeoxygenation. The optimized Rh@Al2.0–mSiO2 catalyst displayed significantly enhanced guaiacol activity and cyclohexane selectivity relative to the Rh@mSiO2 catalyst under mild reaction conditions. According to the characterization results, the high hydrodeoxygenation activity of Rh@Al2.0–mSiO2 could be attributable to the synergistic effect between the metallic Rh and Lewis and Brønsted acid sites, and the introduction of Al species greatly facilitated the adsorption of 2-methylcyclohexanol, thereby enhancing cyclohexane selectivity. The confinement effect of Rh NPs inside the hollow cavities effectively prevents the leaching and aggregation of Rh NPs, thereby improving their catalytic durability and stability.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Qiang Li,Mingjun Huang,Fucheng Li,Zhe Ling,Yao Meng,Fushan Chen,Zhe Ji,Songlin Wang
The preparation of degradable, stable, acid- and alkali-resistant oil/water separation materials from renewable biomass resources is a vast challenge as well as vital for sustainable development. Inspired by the asymmetric wettability of lotus leaf, a brand-new type of cellulose-based Janus paper sheets with anisotropic wettability was successfully designed and engineered with industrial lignin residues and nano-silica. By easy spraying of coatings to construct hierarchical networks, the papers achieved robust superhydrophobicity in a variety of acidic and alkaline conditions (pH = 3–11) with a water contact angle about 153°. Benefiting from the lipophilicity of lignin and the hydrophilicity of cellulose, Janus paper sheets were endowed an excellent oil-water separation efficiency. It reached a maximum flux of 654.46 L·m −2 h −1 of dichloromethane in the solvent-water mixture. Furthermore, the mechanical properties, folding and tearing resistance of the obtained materials were significantly improved due to the splendid interfacial adhesion, rendering them satisfied stability and durability. The oil-water separation efficiency of the Janus paper sheets was maintained at 90% over 8 recycles. In contrast to cumbersome oil-water separation materials, the proposed Janus paper sheets can operate as an efficient, stable, acid- and alkali-resistant, abrasion-resistant biodegradable material to effectively absorb heavy oils and waste organic solvents. A novel application possibility is provided by such an environmentally friendly, reliable, and efficient preparation process for oil-water separation.
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 22
·7493
·
IF 4.6
Hujun Niu,Xudong Chen,Yunbo Zhao,Junyi Zhou,Yimin Xie
To further our understanding of the change in association between lignin and carbohydrates after kraft pulping, isotope-labeled kraft pulp (KP) was prepared using13C and D double-isotope-labeled wheat straw, and it was subjected to enzymatic hydrolysis and ionic liquid treatment to explore the linkages between lignin and carbohydrate complexes in wheat straw. Isotope abundance determination showed that13C and D abundances in the experimental groups were substantially higher than those in the control group, indicating that the injected exogenous coniferin-[α-13C], coniferin-[γ-13C], andd-glucose-[6-D2] were effectively absorbed and metabolized during wheat internode growth. Solid-state CP/MAS13C-NMR spectroscopy showed that lignin was mainly linked to polysaccharides via acetal, benzyl ether, and benzyl ester bonds. Kraft pulp (KP) from the labeled wheat straw was degraded by cellulase. The obtained residue was fractionated using the ionic liquid DMSO/TBAH to separate the cellulose–lignin complex (KP-CLC) and xylan–lignin complex (KP-XLC). X-ray diffractometer determination showed that the KP-CLC regenerated cellulose type II from type I after the ionic liquid conversion. The13C-NMR spectrum of Ac-En-KP-CLC showed that the cellulose–lignin complex structure was chemically bonded between the lignin and cellulose through acetal and benzyl ether bonds. The13C-NMR spectrum of En-KP-XLC showed a lignin–hemicellulose complex structure, wherein lignin and xylan were chemically bonded by benzyl ether and acetal bonds. These results indicate that the cross-linking between lignin and carbohydrates exists in lignocellulosic fibers even after kraft pulping.Keywords:wheat straw;lignin–carbohydrate complex;isotope tracer;kraft pulping;ionic liquid
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Ying Kang,Xingmei Lu,Junli Xu,Qing Zhou,Guangjin Zhang,Jiayu Xin,Dongxia Yan,Ibrahim E.I. Tantawy E.I. Sayed
Transforming lignin into aromatic monomers is critically attractive to develop green and sustainable energy supplies. However, the usage of the additional catalysts like metal or base/acid is commonly limited by the caused repolymerized and environmental issues. The key step is to mediate electron transfer in lignin to trigger lignin C-C/C-O bonds cleavage without the catalysts mentioned above. Here, we report that the ionic liquids [BMim][ClO 4 ] was found to trigger lignin electron transfer to cleave the C-C/C-O bonds for aromatic monomers without any additional catalyst. The proton transfer from [BMim] + to [ClO 4 ] − could polarize the anion and decrease its structure stability, upon which the active hydroxyl radical generated and induced lignin C-C/C-O bonds fragmentation via free radical-mediated routes with the assistance of photothermal synergism. About 4.4 wt% yields of aromatic monomers, mainly composed of vanillin and acetosyringone , are afforded in [BMim][ClO 4 ] under UV-light irradiation in the air at 80 °C. This work opens the way to produce value-added aromatic monomers from lignin using an eco-friendly, energy-efficient, and simple route that may contribute to the sustainable utilization of renewable natural resources.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Communications
·
2023
·
IF 3.8
Ruoning Chu,Xiaojie Guo,Yongjun Zhang,Xiaoyu Zhao,Xiantao Xiong,Xiujuan Zhang,Fengyi Zhang,Kun Zhang,Yaxin Wang
Water containing heavy metal ions can be extremely harmful to the environment and human body, thus the development of low-cost and high-efficient adsorbents has an exciting prospect. In this study, lignin/graphene aerogels modified with polydopamine and polyethyleneimine , respectively, were successfully prepared to remove Cr(VI) from aqueous waste. The physicochemical properties of graphene aerogels (GA), lignin/graphene aerogels (LGA), polydopamine-modified lignin/graphene aerogels (LGA@PDA), polyethyleneimine-modified lignin/graphene aerogels (LGA@PEI) were investigated using FT-IR, Raman spectroscopy , XRD , XPS , SEM-EDS, and BET analysis. The results demonstrate that adsorbents have a high specific surface area, an interconnected porous structure, and a large number of oxygen-containing groups, making them particularly favorable for heavy metal adsorption. The effects of GO/lignin ratio, surface modifiers, solution pH, contact time, initial concentration and temperature on the Cr(VI) removal were investigated and compared via batch experiments. Compared with GA (138.74 ± 3.93 mg/g), the adsorption capacity of LGA with GO/LA ratio 40:1 increased to 167.66 ± 4.75 mg/g. Furthermore, the maximum adsorption capacity of LGA@PEI and LGA@PDA rose up to 209.85 ± 3.25 mg/g and 240.39 ± 3.26 mg/mg, respectively. By simulating the experimental data with different kinetic models and isotherm models, the adsorption processes of different lignin-derived aerogels were further explored under various conditions. All types of aerogels fit well with the pseudo-second-order model and Langmuir model. In addition, the XPS results confirm that the chemical reduction of Cr(VI) to Cr(III) also plays a role in the removal of Cr(VI). The results demonstrated that the removal effect of lignin-derived aerogels on Cr(VI) was greatly improved through the multi-functionalized surface modification of LGA with PDA and PEI. Furthermore, the removal efficiency of LGA@PDA and LGA@PEI for Cr(VI) remained stable after repeated regeneration. Therefore, the results of this study indicate that LGA@PDA and LGA@PEI are promising Cr(VI) adsorbents for practical applications in wastewater treatment.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Ling Yang,Wenjie Luo,Yassen Muhammad,Fanyu Meng,Jiashun Li,Zhenxia Zhao,Jing Li
Agroforestry solid waste bagasse fiber (BF) possesses sustainable, carbon-neutral characteristics when used as a reinforcement material for asphalt pavements. However, the incompatibility between BF and the asphalt matrix limits its wide application. This study proposes a strategy for cost-effective and environmentally friendly modification of fiber surfaces, aiming to transform a drawback into an advantage. That is, the lignin in BF, which affects the tensile strength of fibers, is dissolved by a deep eutectic solvent (DES) system, and then the lignin is reborn on the surface of the fibers with the assistance of tannic acid . Based on the hydrophobicity and free radical trapping properties of lignin, regenerated lignin is expected to act as a natural coupling agent between BF and styrene-butadiene-styrene (SBS) asphalt materials and as an anti-aging agent for asphalt. The experimental results showed that the modified BF realized the enhancement of asphalt interfacial compatibility and toughening of asphalt matrix. Specifically, the shear resistance, viscoelasticity and rutting resistance of the modified BF/SBS-modified asphalt were improved by 46.61%, 22.67% and 30.06%, respectively, and the UV aging susceptibility was decreased by 75.02% compared with that of the BF/SBS-modified asphalt. In conclusion, this work introduces a simple and practical strategy for enhancing the interaction between BF and asphalt, which is crucial for advancing biomass recycling and green transportation development.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Jianming Tao,Zicong Hu,Qian Ma,Caiqiong Zhou,Lin Lei,Guohua Zhao
The widespread environmental heavy metal , Pb, is renowned for inducing irreversible damage to human health. Lignin, an original fiber, emerges as a promising natural candidate for mitigating lead toxicity owing to its exceptional adsorption capacity and biocompatibility. In this study, we conducted an investigation into the potential therapeutic effects of lignin derived from the bamboo ( Dendrocalamus Latiforus ) shoot shell (BSS-AAL) in alleviating Pb-induced oxidative stress and hypercholesterolemia in hamsters. Our findings demonstrated the remarkable ability of BSS-AAL to reduce Pb accumulation by 27–40% in plasma and 13–84% in tissues. Furthermore, BSS-AAL exerted reparative effects on the antioxidant system, evidenced by substantial reductions in plasma total cholesterol levels by at least 35% and hepatic cholesterol levels by an impressive 66%. Intervention with BSS-AAL also led to favorable alterations in the richness of key microbial genera, including norank_f__Erysipelotrichaceae , unclassified_f__Atopobiaceae , and norank_f__Eubacteriaceae , which are associated with modulating malonaldehyde accumulation, hepatic cholesterol 3-hydroxy-3-methylglutaryl coenzyme A reductase activity, as well as short chain fatty acids synthesis. These findings substantiated BSS-AAL played a vital role in effectively modulating Pb-induced oxidative stress and hypercholesterolemia by reducing Pb accumulation and favorably influencing gut microbiota.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）