COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Mingen He,Hang Wang,Jiamei Yang,Fuxiang Chu,Yiqiang Wu,Fuquan Xiong
Flexible supercapacitors combine the advantages of conventional supercapacitors, including excellent mechanical properties, stretchability, and bendability, making them crucial components in wearable electronic devices. Herein, nitrogen and phosphorus co-doped lignin-derived carbon nanosphere (NPCS)/reduced graphene oxide (rGO) flexible electrode materials were synthesized through vacuum filtration and reduction methods. With increasing mass ratio of carbon nanospheres, the electrochemical performance of the electrode gradually improved, reaching an outstanding capacitance of 174.6 F g −1 for a 1:1 ratio of NPCS to rGO at 1 A g −1 . Additionally, the electrode maintained stable performance even after bending at different angles. The electrode, assembled into a symmetric supercapacitor with a 6 M KOH electrolyte, exhibited an outstanding capacitance of 130.5 F g −1 at 1 A g −1 and exceptional cycle stability, retaining 98.05% of its original capacitance after 5000 cycles at 5 A g −1 . At a power density of 49.52 W/Kg, the electrode exhibited an energy density of 5.03 Wh/Kg. Moreover, the electrode maintained an excellent capacitance of 143.0 F g −1 in an acidic electrolyte (1 M H 2 SO 4 ) at 1 A g −1 . However, the electrode exhibited reduced capacitance in a neutral electrolyte (1 M Na 2 SO 4 ) but achieved a significantly higher energy density of 22.3 Wh/kg. The flexible electrode material exhibited adaptability to different acid–base conditions and maintained good flexibility, highlighting its significant potential for development in flexible supercapacitors.
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GREEN CHEMISTRY
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2025
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IF 9.2
Hanwen Ge,Jiahui Wei,Shenglin Wang,Zexu Yan,Jiang Mingzhe,Lingxiao Zhu,Chao Liu,Bin Li,Caoxing Huang,Huanfei Xu
Heightened requirements in terms of environment, economy, and efficiency had been imposed on solvents used in the treatment of lignocellulose by the upgrading of the concept of green chemistry. Limitations were imposed on studies that only focus on enhancing a single interaction within the system due to the lack of understanding of the molecular-level mechanism in the solvent-biomass system. In this work, four novel ternary deep eutectic solvents (DES) were synthesized by adopting a new strategy in which the synergistic effect of hydrogen bonds (H-bonds), van der Waals (vdW) interactions and π-π stacking was used to enhance the delignification ability of DES. It was indicated by the results of quantum chemical calculation based on density functional theory (DFT) and molecular dynamics (MD) simulation that 84.26% and 68.72% of the electrostatic energy and vdW interaction energy in the DES-Lignin system were contributed, on average, by choline chloride (ChCl) and p-hydroxybenzoic acid (PB), with increases of 21.60% and 27.71% successively. This improvement was attributed to the increased molecular polarity resulting from the N⁺ on ChCl, the enhanced dispersion attraction due to the arrangement of methyl groups around the sp³-hybridized N⁺, and the π-π stacking interaction formed between the benzene ring structure of PB and lignin, which resulted in the enhancement of vdW interaction within the system. Affected by the ortho-substituents on the benzene ring, among the six investigated lignin dimers, stronger interactions with DES were exhibited by β-1 and β-O-4. The delignification ability of ChCl-LA-PB (strongest calculated interaction energy, reaching -92.37 kcal/mol) was demonstrated in the experiment of treating xylose residue. The delignification rate of lignin was increased by 1.86 times (up to 61.91%) compared with that of ChCl-LA. It was confirmed by the characterization resulted that the excessive depolymerization and condensation of lignin were avoided by the p-π conjugation effect of the phenolic hydroxyl group on PB through inhibiting the ionization of H⁺. Designing DES from the origin of molecular structure and adopting a strategy of multiple interactions in synergy provided novel insights and green methods for the high-value utilization of lignocellulose.
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SEPARATION SCIENCE AND TECHNOLOGY
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2025
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IF 2.3
Zhiyi Wang,Hongjuan Bai,Zifan Liu,Zihan Jin,Jing Lv,Ziyu Zhang,Le Wang
This study investigates the adsorption performance of humic acid-functionalized lignin-based microspheres (HA@LGMS) in eliminating Acid Orange 7 (AO7) and tetracycline (TC) contaminants from wastewater. Lignin, a residual material from pulp manufacturing processes, was utilized to synthesize lignin-based microspheres (LGMS) via reversed-phase suspension polymerization. Subsequently, humic acid was incorporated into LGMS to enhance their adsorption capacity. Comprehensive material characterization involving SEM, FTIR, XPS, etc. revealed the structural features and surface chemistry of the microspheres. Systematic batch adsorption studies examined the adsorption kinetics, isotherms, and thermodynamics of AO7 and TC onto HA@LGMS. Analysis demonstrated chemisorption-driven mechanisms supplemented by boundary layer diffusion and pore penetration phenomena. The adsorption processes were spontaneous and endothermic, with higher temperatures favoring adsorption. HA@LGMS exhibited high adsorption capacities for AO7 (434.81 mg/g) and TC (93.98 mg/g), outperforming many existing adsorbents. The adsorbent also demonstrated excellent reusability and stability in multiple adsorption-desorption cycles. Moreover, HA@LGMS effectively removed AO7 and TC from real water samples, highlighting its potential for practical wastewater treatment applications. This study provides a sustainable and cost-effective solution for the removal of dyes and antibiotics from wastewater using lignin-based materials.
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WOOD SCIENCE AND TECHNOLOGY
·
2025
·Vol. 60
·期 1
·17
·
IF 3
Han Yuchen,Zhong Wei,Zheng Jie,Wu Jianfeng,Jiang Bo,Jin Yongcan,Wu Wenjuan
Lignin possesses the advantages of high carbon content and abundant functional groups, making it suitable as a supercapacitor electrode material. However, the microstructure of lignin-derived electrode materials obtained through traditional methods limits the effective utilization of energy storage capacity, resulting in a significant loss of electrochemical efficiency. Doping with heteroatoms in lignin-derived carbon can enhance its electrochemical performance and is a promising method for performance improvement. We employed a green and universal approach to design lignin-derived carbon materials by covalently grafting phosphorus source (DOPO) and nitrogen source (HDI) onto the lignin macromolecular framework through organic synthesis. Using modified lignin (NPAL) as a precursor, we achieved simultaneous carbonization and activation through a one-pot method. The nitrogen and phosphorus doping synergistically enhances pseudocapacitance activity (redox reactions), optimizes the hierarchical pore structure (increasing the specific surface area to 1756.79 m 2 /g), and improves charge transfer kinetics (reducing charge transfer resistance to 6.63 Ω). This results in a high specific capacitance (276.3 F/g @ 0.25 A/g, an increase of 275.56% compared to undoped materials), high energy density (12.5 Wh/kg), and cycling stability (capacity retention of 92.5% after 10,000 cycles), indicating a promising application prospect.
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ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Jing Bai,Yang Zhang,Xinghua Zhang,Chenguang Wang,Longlong Ma
High-density polycyclic alkanes prepared from lignocellulose biomass are an important substitute for fossil fuels. Here, we reported a synthesis strategy in that lignin-derived phenol and benzyl acetate were used to synthesize jet fuel-range high-density alkanes. Benzylphenols (C13-oxygenated compounds) were synthesized through the alkylation reaction of phenol and benzyl acetate over a montmorillonite (MMT) catalyst. The lewis acid site of MMT is favorable for the formation of the benzyl cation, promoting the alkylation reaction. Under the conditions of 140 °C and 2 h, the yield of alkylation products reaches 70%. Subsequently, the hydrodeoxygenation (HDO) of alkylation products was conducted over a 5 wt % Pd/C catalyst, and the yield of 85% hydrocarbons was obtained. Perhydrofluorene and dicyclohexylmethane were the dominant components in the HDO products. The density and heating values of HDO products were 0.956 g/cm3 and 38.9 MJ/L, respectively.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Yuqing Liang,Hanwen Zuo,Mingyu Wen,Junyou Shi,Heejun Park
The traditional epoxy resin not only is flammable and non-recyclable and but also heavily dependents on petroleum resources, which cannot meet the requirements of fire prevention and sustainable development. In this study, a vanillin intermediate (VAP) with dynamic imine bond (C=N) was prepared by schiff base reaction between the lignin derivative vanillin (-CHO) and the cage-like polyhedral oligomeric silsesquioxane OA-POSS(−NH 2 ). Then, a biomass-based P-N-Si flame retardant (VAPD) was synthesized by adding 9,10-Dihydro-9-Oxa-10-Phosphaphenanthrene-10-Oxide (DOPO) into the VAP. Subsequently, the VAPD acted as curing agent of epoxy resin to prepare epoxy wood coatings (VAPDs/EP). The results showed that the VAPD-5/EP coating not only exhibited excellent self-healing property and was able to achieve 100 % healing within 35 min, but also presented distinctive UV-shielding performance. In addition, the VAPD-5/EP coating reached V-0 level of UL-94 test and got 29.3 % of limiting oxygen index (LOI). Compared with EP coating, the peak heat release rate (pHRR) decreased by 38 %. Furthermore, the VAPD-5/EP coating reached 6H level of hardness test and 4B level of adhesion test. A simple strategy for preparing self-healing flame retardant epoxy coatings with comprehensive properties for protection of wood materials was proposed in this study.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Haibin Ji,Somia Yassin Hussain Abdalkarim,Yunfei Shen,Xuefei Chen,Yixuan Zhang,Jiayuan Shen,Hou-Yong Yu
Biomass-based slow-release fertilizers (SRFs) are a sustainable solution for addressing food scarcity, improving fertilizer efficiency, and reducing pollution, whereas they still face complex preparation, high costs, and low release characteristics. This study introduces a simple and innovative approach to producing bifunctional green SRFs with controlled release and conditioning properties for saline soils and harsh environments. The method involves a one-pot preparation of microsphere-structured amine-modified lignin slow-release fertilizer (L-U X ) using biomass lignin as the starting material. The L-U X demonstrates an exceptional fertilizer loading rate (66.2 %) and extended slow-release performance (288 h), effectively enhancing the fertilizer's release ability. Compared to traditional fertilizers, the bifunctional L-U X significantly improves soil water retention capacity (824.3 %), plant growth, and germination percentage in challenging soil conditions (133 %). These findings highlight the potential of L-U X as a large-scale controlled-release fertilizer in harsh environments. A life cycle assessment (LCA) was also conducted to evaluate the environmental impact of L-U X from its production to disposal. This revealed that L-U X has a minimal environmental footprint compared to conventional inorganic fertilizers. This study further supports the widespread application of L-U X as an environmentally friendly alternative.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 1
·016504
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IF 4.316
Haomin Jiang,Yujuan Cheng,Zhaohui Wang,Zhiqun Bai,Yang Tang,Yanzhi Sun,Pingyu Wan,Yongmei Chen
The cleavage of the linkage bonds among the C9 units in lignin molecules via selective oxidation method to obtain small-weight aromatic compounds is an important way to lignin valorisation. In this study, the cleavage pathways of bonds in a lignin model compound, GGE (guaiacylglycerol-β-guaiacyl ether), by the reactive oxygen species (ROS) in situ generated through electrochemical oxygen reduction reaction (ORR) in an aprotic ionic liquid ([BMIM]BF4) was investigated. The results indicated that when the main ROS was ·OOH, coniferyl alcohol, guaiacol and vanillin were detected as the degradation products which is supposed to be caused by β-O-4 bonds cleavage; Otherwise, when HO2− was the main ROS, coniferyl alcohol could not be detected and the degradation reaction is believed to be trigerred by Cα-Cβ bonds cleavage.
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Bioresource Technology Reports
·
2023
·
IF 0
Shaoqing Wang,Gaixiu Yang,Juntao Yang,Zhen Wan,Zhihe Li,Weiming Yi
In this paper, the ternary molten salt (Li 2 CO 3 -Na 2 CO 3 -K 2 CO 3 ) was introduced into the lignin pyrolysis process for the co-production of monophenols and value-added carbon materials. The effect of lignin/molten salt ratios (i.e., 3:1, 1:1, and 1:3) on lignin pyrolysis behaviour was investigated herein. The pyrolytic products were characterized by gas chromatography–mass spectrometry, ultimate analyses, scanning electron microscopy, nitrogen adsorption analyses, and Raman analyses. Results showed that molten salt media can promote the conversion of bulky phenolic oligomers into mono-phenols by enhancing the cracking and deoxygenation reactions. P-type phenols (49.76 %) were produced when the lignin/molten salt mass ratio was 1:3. The porosity and aromaticity of biochar were regulated in-situ using molten salt. The possible catalytic effect of molten salt on lignin pyrolysis was proposed. This study provides a case reference for lignin waste resource utilization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiao Han,Mooeez Ur Rehman,Junhu Wang,Alexandre Rykov,Oliver Y. Gutiérrez,Yujun Zhao,Shengping Wang,Xinbin Ma,Johannes A. Lercher
The catalytic hydrodeoxygenation (HDO) of lignin-derived phenolic compounds is a critical step in the upgrading of bio-oil. Here, bimetallic Ni-Fe nanoparticles supported on mesoporous carbon spheres (MCSs) were fabricated and applied in HDO of phenol. In comparison with monometallic Ni and Fe catalysts, the bimetallic Ni-Fe catalyst exhibited better performance for phenol HDO due to the formation of Ni-Fe alloy phase identified by X-ray powder diffraction (XRD) and Mössbauer spectroscopy techniques. Among several explored ratios, the catalysts with Ni/Fe ratio of 3/1 presented the highest cyclohexane yield. The reaction occurred in two consecutive steps: the hydrogenation of phenol to cyclohexanol and the further hydrogenolysis of cyclohexanol to cyclohexane. Kinetic studies showed that the hydrogenolysis of cyclohexanol controlled the overall reaction rate of phenol HDO due to the lower reaction rate of this step. Indeed, the turnover frequency (TOF) values of cyclohexanol normalized by surface metallic Ni sites exhibited a linear correlation with Ni-Fe alloy sites. The alloying of iron in the bimetallic Ni-Fe catalysts significantly enhanced the adsorption strength of cyclohexanol, which is the reason of the high activity of the Ni-Fe alloy particles. Thus, Fe-containing sites adsorb the hydroxyl species while Ni sites perform the H 2 activation, their synergistic effect plays a key role in phenol HDO process.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·Vol. 28
·期 7
·2021-2033
·
IF 2.5
Duan Yuting,Long Jiadong,Li Yanhang,Tian Xin,Li Jiaqi,Fang Zezhong,Wang Jian,Huo Pengfei
Owing to the increasing low-carbon demand, environmentally friendly supercapacitors with low temperature resistance have attracted increasing attention. Herein, biomass hydrogels were successfully fabricated by covalently cross-linked lignin (Lig) with soy protein isolate (SPI) and assembled into supercapacitors. The performance of hydrogel electrolytes and the electrochemical performance of supercapacitors were studied systematically. The hydrogel electrolyte achieved the highest ionic conductivity of 0.086 S cm −1 with 50% addition of SPI. The supercapacitor displayed an excellent specific capacitance of 150.80 F g −1 at room temperature. Importantly, over 10,000 charge-discharge cycles, the capacitance retention rate maintained more than 73.5%, and the coulombic efficiency was around 100%. Besides, the electrochemical performance of the supercapacitors at low temperature was investigated as well. Even at −20 °C, the flexible supercapacitor could keep a specific capacitance of 135.71 F g −1 , with a capacitance retention rate up to 90% of room temperature, indicating a prominent resistance at subzero temperature. Overall, this work lays a foundation for the preparation of environmentally friendly and low temperature resistant solid-state supercapacitors, which is conducive to the practical application under harsh environments. Graphical
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BIORESOURCE TECHNOLOGY
·
2020
·
IF 7.539
Qingfeng Liu,Yunfei Bai,Hong Chen,Mengmeng Chen,Yushuai Sang,Kai Wu,Zewei Ma,Yiming Ma,Yongdan Li
The efficient depolymerization and hydrodeoxygenation of enzymatic hydrolysis lignin are achieved in cyclohexane solvents over a gamma-alumina supported nickel molybdenum alloy catalyst in a single step. Under initial 3 MPa hydrogen at 320 °C, the highest overall cycloalkane yield of 104.4 mg/g enzymatic hydrolysis lignin with 44.4 wt% selectivity of ethyl-cyclohexane was obtained. The reaction atmosphere and temperature have significant effects on enzymatic hydrolysis lignin conversion, product type and distribution. The conversion of enzymatic hydrolysis lignin was also investigated over different nickel and molybdenum-based catalysts, and the gamma-alumina supported nickel molybdenum alloy catalyst exhibited the highest activity among those catalysts. To reveal the reaction pathways of alkylphenol hydrodeoxygenation, 4-ethylphenol was tested as a model compound. Complete conversion of 4-ethylphenol into cycloalkanes was achieved. A two-step mechanism of 4-ethylphenol dihydroxylation – hydrogenation is proposed, in which the benzene ring saturation is deemed as the rate-determining step.
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