CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xuan Zhou,Can Jin,Guifeng Liu,Guomin Wu,Shuping Huo,Zhenwu Kong
With the increasing concern in sustainable development and environmental governance, the biomass-based magnetic materials containing sufficient active sites and regular structure can be regarded as the high-performance adsorbents for removal of heavy metal pollutants from wastewater. In this study, we reported the tunable covalent binding of lignin onto amine-functionalized magnetic nanoparticles (AMNP) using cyanuric chloride as a chemoselective cross-linker. The chemical structures, morphologies, and magnetic properties of the synthesized lignin-based magnetic adsorbents (L1@MNP and L2@MNP) were comprehensively characterized. Batch adsorption experiments were conducted to investigate various effecting factors, including pH, contact time, solution concentration and temperature. With the higher component ratio of AMNP/lignin, L1@MNP displayed higher adsorption affinity ( q max = 111.23 mg/g) and selectivity towards Pb(II) than L2@MNP ( q max = 81.97 mg/g). The adsorption kinetics agreed well with the pseudo-second-order kinetic model, and the thermodynamic adsorption behaviors were found to be an endothermic and spontaneous process. In addition, the presence of magnetic cores in the network facilitated the fast recovery of both two magnetic adsorbents after the adsorption process, owing to the good superparamagnetic properties for L1@MNP (40.06 emu/g) and L2@MNP (26.95 emu/g). Furthermore, the core–shell magnetic adsorbents also showed superior stability even in an acidic solution, of which the removal efficiency could well maintain over 85% after 5 cycles. This work provides a facile strategy for the design and synthesis of lignin-based adsorbents with flexible nanoparticles as a building block for the potential application prospects in Pb(II) removal from wastewater.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Qinhua Wang,Jinxin Lan,Zifeng Hua,Xiaojuan Ma,Lihui Chen,Xiaofeng Pan,Yang Li,Shilin Cao,Yonghao Ni
The development of conductive, soft, ultra-stretchable, and asymmetrically adhesive hydrogels is difficult and essential for both wearable electronics and anti-adhesion tissue dressings. In particular, there is still no simple, effective and universal approach to construct an asymmetrically adhesive multifunctional hydrogel. Here, we first synthesized lignosulfonate sodium (LS)-doped PAA hydrogels with uniform adhesion (adhesive strength : ~30.5 kPa), conductivity (~0.45 S/m), stretchability (up to ~2250%), and low compressive modulus (~20 kPa). In the second step, an oriented soaking of Fe 3+ onto the upper surface of the resultant composite hydrogel renders the upper surface non-adhesive. This novel strategy masterfully delivers asymmetric adhesion behavior to the upper and bottom surfaces of the same hydrogel (~0 kPa adhesive strength for the upper surface; strong adhesive strength of ~27 kPa for the bottom surface). The asymmetric adhesive hydrogel has proven to adhere well onto the human skin and achieve waste-barrier. Importantly, this hydrogel assembled pressure sensor demonstrates excellent anti-interference and wearable comfort.
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Journal of Environmental Chemical Engineering
·
2022
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IF 7.968
Junwang Zhang,Xinyu Zhu,Xiaoxiao Xu,Qingqin Sun,Ligang Wei,Kunlan Li,Shangru Zhai,Qingda An
The oxidative depolymerization of alkali lignin can be achieved by using Keggin structure polyoxometalate-ionic liquid (POM-IL) as catalyst under aerobic conditions . The effects of catalysts such as [HC 4 im] 3 PMo 12 O 40 , [HC 4 im] 5 PV 2 Mo 10 O 40 , [HC 2 im] 5 PV 2 Mo 10 O 40 , and [HC 4 im] 4 SiMo 12 O 40 (abbreviated as POM-IL1, POM-IL2, POM-IL3, and POM-IL4, respectively), the acidity of aqueous IL solutions on lignin conversion, and aromatic product distribution were investigated. Under optimized conditions, phenolic products (mainly m (p)-cresol, veratrole, vanillin) had the highest yield and the selectivity was as high as 75.0% using POM-IL1 as the catalyst. POM-IL2 and POM-IL3 were used as the catalysts, the highest conversion of 76.0% of lignin was achieved, and the overall yield of ketone products were higher on lignin samples, in which the main products include acetovanillone, 3-methoxyphenol, and 4-methylcatechol, and the highest selectivity of ketone products was 76.8%. The results show that the lignin fragments could be successfully oxidized into platform compounds in aqueous acidic ILs (AILs) solutions catalyzed by Keggin structure POM-IL. In addition, the role of AILs and POM-ILs in the oxidative depolymerization of alkaline lignin was analyzed, and the possible reaction mechanism between AIL-water/POM-IL/lignin system was speculated.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2024
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IF 9.7
Pengfei Zhao,Fulong Pu,Changsheng Su,Yefan Wan,Texin Huang,Xuedan Hou,Di Cai
Deep eutectic solvents (DESs) offer a potential opportunity in biomass utilization industries. This work emphasized the impact of hydrogen bond donors (HBD) and acceptors (HBA) on deconstruction and valorization of rice straw. Acidity, alkyl chain length, hydrogen bonding ability and functional groups of HBD and HBA appeared to be important factors affecting the fractionated pulps and lignins, which further influenced ethanol fermentation. Among the candidate DESs, lactic acid/guanidine hydrochloride (LGH) was proved to be the most suitable one due to the excellent delignification and xylan removal. For the downstream fermentation process, 0.47 g g −1 of bioethanol with 0.55 g/L h −1 of productivity can be obtained from the LGH pulp’s hydrolysate. Mass balance showed 302.8 g bioethanol and 119.0 g technical lignin can be co-generated from 1 kg dried rice straw. This “green” valorization strategy offers a promising scheme in biorefinery of lignocelluloses.
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Fangbao Fu,Dongjie Yang,Bowei Zhao,Yukang Fan,Weifeng Liu,Hongming Lou,Xueqing Qiu
Heteroatom-doped porous carbon materials show promise for use as supercapacitor electrodes, but the tradeoff between surface area and the heteroatom dopant levels limits the supercapacitive performance. Here, we modulated the pore structure and surface dopants of N, S co-doped hierarchical porous lignin-derived carbon (NS-HPLC-K) via self-assembly assisted template-coupled activation. The ingenious assembly of lignin micelles and sulfomethylated melamine into a magnesium carbonate basic template greatly promoted the KOH activation process, which endowed the NS-HPLC-K with uniform distributions of activated N/S dopants and highly accessible nanosized pores. The optimized NS-HPLC-K exhibited a three-dimensional hierarchically porous architecture composed of wrinkled nanosheets and a high specific surface area of 2538.3 ± 9.5 m 2 /g with a rational N content of 3.19 ± 0.01 at.%, which boosted the electrical double-layer capacitance and pseudocapacitance. Consequently, the NS-HPLC-K supercapacitor electrode delivered a superior gravimetric capacitance of 393 F/g at 0.5 A/g. Furthermore, the assembled coin-type supercapacitor showed good energy-power characteristics and cycling stability. This work provides a novel idea for designing eco-friendly porous carbons for use in advanced supercapacitors.
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APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Linhuo Gan,Li Lyu,Tianruo Shen,Shuai Wang
Sulfonic acid-functionalized lignin-derived mesoporous carbon (LDM C-S O 3 H) was prepared using phenolation and evaporation induced self-assembly method followed by sulfonation. The obtained LDM C-S O 3 H bearing sulfonic acid density of 0.6528 mmol/g possessed a well-ordered two-dimensional hexagonal mesoporous characteristics. A 5-hydroxymethylfurfural (5-HMF) yield of 98.0% with a full fructose conversion was obtained using LDM C-S O 3 H as catalyst at 140 °C for 2 h in DMSO. Reactive kinetics studies revealed that fructose conversion in DMSO without catalyst or catalyzed by LDMC-SO 3 H may obey pseudo-first-order kinetics, and the activation energy of latter (72 kJ/mol) was much lower than that of former (114 kJ/mol). Adsorption kinetics studies indicated that almost no 5-HMF adsorbed onto LDM C-S O 3 H probably had a great contribution to the high selectivity of up to 98.0%, while the fructose adsorption on LDM C-S O 3 H was a diffusion-controlling adsorption process with more following Bangham kinetic model and Weber-Morris kinetic model owing to the characteristics of ordered mesostructure of LDM C-S O 3 H. Moreover, LDM C-S O 3 H exhibited superior reusability and stability in catalytic performance with a 5-HMF yield higher than 88.0% in six runs probably due to the synergistic effect of mesopore structure with a special surface and -SO 3 H groups with a relatively high content. These research results will contribute to a better understanding of structure-performance relationship of LDM C-S O 3 H used as an efficient catalyst in the fructose-to-5-HMF transformation as well as the high-value utilization of lignin in the field of catalysis.
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高影响因子
BIORESOURCE TECHNOLOGY
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2017
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IF 5.651
Jindong Wang,Wenzhi Li,Huizhen Wang,Qiaozhi Ma,Song Li,Hou-min Chang,Hasan Jameel
In this study, a novel catalyst, S 2 O 8 2− -KNO 3 /TiO 2 , which has active acidic and basic sites, was prepared and used in lignin hydrocracking with a co-catalyst, Ru/C. Ru/C is an efficient hydrogenation catalyst and S 2 O 8 2− -KNO 3 /TiO 2 is a dual catalyst, which could efficiently degrade lignin. This catalytic hydrogenation system can reduce solid products to less than 1%, while giving a high liquid product yield of 93%. Catalytic hydrocracking of kraft lignin at 320 °C for 6 h gave 93% liquid product with 0.5% solid product. Most of this liquid product was soluble in petroleum ether (60% of 93%), which is a clear liquid and comprises mainly of monomeric and dimeric degradation products . These results demonstrated that the combination of the two catalysts is an efficient catalyst for liquefaction of lignin, with little char formation (∼1%). This concept has the potential to produce valuable chemicals and fuels from lignin under moderate conditions.
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高影响因子
Molecular Catalysis
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2021
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IF 5.062
Yuchen Zhu,Hao Wu,Zheng Fang,Xiaobing Yang,Kai Guo,Wei He
Cobalt (II)-meso-tetra(4-carboxyphenyl) porphyrin supported by deprotected lignin was synthesized through the covalent linkage between carboxy groups in the porphyrin and hydroxyl groups in the lignin. The resulting supporting catalysts were applied in the selective oxidation of 5-hydroxymethylfurfural. Through solvent optimization, 5-hydroxymethyl-2-furancarboxylic acid and 2,5-furandicarboxylic acid could be selectively obtained. Steric effect of lignin prevented unwanted aggregation-caused quenching, avoiding catalyst deactivation. Thus, supported catalysts displayed better catalytic efficiency compared free metal porphyrin catalyst. Unlike the excessive use of sodium hydroxide in the oxidation of HMF catalyzed by metal catalysts, an equivalent amount of sodium hydroxide was used in this oxidation process. Meanwhile, lower activation energy was detected when metal porphyrin supported by deprotected lignin was used. By adjusting the pH in the reaction, supported catalysts could be reused. The catalytic activity remained stable during the recycling experiments.
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COMBUSTION AND FLAME
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2020
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IF 4.57
Qiang Lu,Wen-luan Xie,Bin Hu,Ji Liu,Wei Zhao,Bing Zhang,Ti-peng Wang
Pyrolysis of lignin involves complex unimolecular decomposition and bimolecular interaction mechanisms. Unimolecular decomposition of lignin model compounds has been widely investigated, while bimolecular interactions are far from well elucidated. Currently, only two radical reaction-based interactions, i.e., hydrogen abstraction and hydrogen-bond-induced homolysis mechanisms, have been proposed to explain the interactions in the lignin pyrolysis process, which ignores the concerted reaction-based interactions involving the pyrolytic products of lignin. Particularly, a large number of phenolics are produced in the pyrolysis of lignin, which can further affect the concerted pyrolysis reactions of lignin. In the present work, a novel interaction mechanism, phenolics-assisted hydrogen transfer (phenolics-AHT) process for the concerted reactions, is confirmed and carefully investigated. Phenylethyl phenyl ether (PPE), a typical β -O-4 lignin dimer, is used as the model compound to reveal the phenolics-AHT mechanism in the lignin pyrolysis system. Density functional theory (DFT) calculation, electrostatic potential (ESP) analysis, and fast pyrolysis experiment results are combined to reveal that the phenolic products participate in the hydrogen transfer process of the concerted Maccoll elimination reaction by means of their phenolic hydroxyl structures and significantly reduce the energy barrier, thus promoting the cleavage of the β -O-4 linkage. On the contrary, phenolics-AHT has no obvious effect on the concerted retro-ene fragmentation. At medium pyrolysis temperatures, the hydrogen transfer processes induced by phenolic products play a more significant role in the dissociation of the β -O-4 linkage than the hydrogen abstraction induced by radicals, due to the limited amount of free radicals . In addition, DFT calculation results further suggest that decarbonylation , decarboxylation , dehydration, tautomerism , and other concerted reactions can also be promoted by phenolics-AHT.
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高影响因子
CHINESE CHEMICAL LETTERS
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2013
·Vol. 24
·期 12
·1091-1094
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IF 1.21
Xin-Ping Ouyang,Chun-Lei Liu,Yu-Xia Pang,Xue-Qing Qiu
A trimeric lignin model compound composed of α - O -4 and β - O -4 linkages was prepared by the microwave-assisted synthesis, which consisted of three steps: (a) the synthesis of 3-methoxy-4-benzyloxyacetophenone ( 2 ) from acetovanillone ( 1 ), (b) the bromination of compound 2 to produce 3-methoxy-4-benzyloxy- α -bromoacetophenone ( 3 ), and (c) followed by a nucleophilic substitution of compound ( 3 ) to obtain 3-methoxy-4-benzyloxy- α -(3-methoxy-4-(1-propenyl)phenol)-acetophenone ( 4 ). The target product was characterized by MS, 1 H NMR and 13 C NMR spectroscopy. It was found that the trimeric compound synthesized can be used as a preferable lignin model compound because it contains guaiacyl structural unit (3-methoxy-4-hydroxy phenyl propane) linked by α - O -4 and β - O -4 linkages. In addition, under the conditions of microwave irradiation, the reaction time of each step is significantly reduced, and the selectivity of target product is greatly improved. The yields of each step and the overall sequence are 95.31%, 87.3%, 90.6% and 75.4% (95.31% × 87.3% × 90.6%), respectively.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Yiping Jin,Zhongwen Zhou,Zekai Yuan,Runjia Hu,Tianran Zhang,Siji Chen,Guang Chen
In this study, straw lignin was separated from corn straw by combining microbial treatment with ρ-TsOH organic acid extraction for the first time, and lignin-derived biochars were prepared by carbonation-activation. The results showed that the extraction rate of lignin and the physicochemical properties of related biochars were improved greatly by microbial treatment. The specific surface areas of lignin biochar obtained after combined pre-treatment with Aspergillus niger , Myrothecium verrucaria , and Trichoderma reesei , (BNL, BML, and BTL) were 2348, 2849 and 3008 m 2 g −1 , respectively, and the total pore volumes were 0.8989, 0.9411, and 1.2621 cm 3 g −1 , which were significantly higher than the 2292 m 2 g −1 and 0.7786 cm 3 g −1 of the control group BCL (biochar prepared from lignin extracted from raw straw). In adsorption experiments by using tetracycline hydrochloride and sodium sulfadiazine as antibiotic models, the maximum adsorption capacities of all lignin-derived biochars (BML, BTL, and BNL) were greater than that of most other adsorbents including BCL. We hope this work could provide a new strategy for efficiently using microbial treatment technology to improve the conversion of lignocellulosic resources.
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产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
He Wan,Yang Liu,Chunhui Yu,Kuiyuan Cao,Yongwei Han,Zhong Sun,Junyou Shi,Xixin Duan
Mild condition and high selectivity are challenging in oxidative depolymerization of lignin to phenolic compounds. In this study, choline chloride (ChCl) was introduced to selectively prepare monophenol compounds from the fractionation of larch lignin with the catalyst of g-C3N4 (CN) supported by H4PMo11VO40 (HPMoV). When the yield of bio-oil was 35%, the novel product of 1-(4-hydroxy-3- methoxyphenyl) butan-1-one (HMB) was obtained with the 11% yield under optimized conditions of 0.2 g 25% HPMoV/CN, ChCl: p-toluene sulfonic acid (PTS) (molar ratio 1:2), 1 mL H2O, 6 h, 80 °C, 220 W xenon lamp and air atmosphere. Results from different deep eutectic solvents (DES) indicated that ChCl was essential for HMB generation. The cleavage of β-O-4 bonds was dominant in the fraction of larch lignin and five representative lignin model compounds (LMCs) under optimum conditions. In addition, distinct degradation mechanisms of native lignin and different LMCs were deduced separately. Compared with other reported products in depolymerizing lignin by chemical oxidative procedures, the presentation of HMB was different because of the conjugate addition of ·CH3 from ChCl accompanying the participation of H2O. Overall, the integrative catalysis from acidic DES, strong oxidizing HPMoV, and visible light in this work provides new insights for valorizing lignocellulose into value-added aromatic products in an ambient, convenient, and photocatalytic reaction system.
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