INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Jianbin Mo,Haochuan Li,Jinxin Yuan,Qiyu Liu,Weifeng Liu,Xueqing Qiu
Polyvinyl alcohol (PVA) is a promising biodegradable and biocompatible polymer material. However, the large number of hydrogen bonds in PVA leads to a contradiction between strengthening and plasticization, which limits its widespread application. To address this challenge, the most abundant aromatic biopolymer, lignin, was adopted as a biobased reinforcing agent for PVA. The simultaneous reinforcement and toughening of PVA by lignin were achieved through the construction of interfacial coordination bonds and hydrogen bonds. The tensile strength and Young's modulus of coordination-reinforced lignin/vanillin-modified PVA (VPVA) composites reached 101 MPa and 1694 MPa, respectively. The thermal processing window of the composites increased from 25.5 °C to 100.5 °C, which provided a potential in thermal processing. Besides, dense hydrogen bonds and coordination bonds conferred good self-healing and water recovery properties onto the composites. Interestingly, the incorporation of lignin also endowed the composites with good photothermal conversion capabilities, making the composites suitable for indoor thermal management. Under simulated solar irradiation of 200 mW/cm 2 , the composites could reduce the indoor temperature rise by 8 °C. This work presents a novel approach for effectively enhancing the comprehensive performance of lignin/PVA composites by coordination bonds, and also presents a pioneering investigation for the high-value utilization of lignin.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Wei Chen,Xinxin Liao,Feng Chen,Xiang Xia,Ping Tong,Yanqiao Jin,Lei Xiong
Considering the facts of fossil fuel depletion and environmental issues, the conversion of biomass into high value-added chemicals is of great importance. In this work, Ni and Co were encapsulated in lignin-derived phenolic resin spheres to obtain NiCo@LRS, which was then employed as a sacrificial template for the synthesis of the bimetallic catalyst NiCo@LC-RS. The Ni and Co act as the acid and dehydrogenation sites for the catalytic transfer hydrogenolysis of 2-phenoxy-1-phenylethanol ( pp-ol ) and corncob lignin, respectively, and exhibit a synergistic enhancement effect. Under the optimal conditions of 170 °C, 1 MPa N 2 and 4 h, the conversion of pp-ol reached 99.9 %, with the yields of cyclohexanol and ethylbenzene at 99.9 % and 93.8 %, respectively. The lignin was completely converted and the selectivity of monophenols was 55.74 %. The catalyst remained stable and reusable after 5 cycles. Furthermore, lignin oil can be employed in the preparation of Ni Co bimetallic catalysts, which have been demonstrated to exhibit excellent catalytic properties. This work provides practical guidance for the high-value utilisation of lignin.
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Food Bioscience
·
2024
·
IF 4.8
Qingsong Zheng,Pamela Owusu Osei,Shaoran Shi,Shuting Yang,Xiaomeng Wu
In this study, we adopted the anti-solvent method to synthesize LNPs using a deep eutectic solvent (DES). We evaluated the dispersibility, particle size, and ζ-potential of the LNPs and observed that they have a particle size distribution of 586–848 nm and showed excellent dispersion and stability. FT-IR and UV were used to demonstrate that the formation mechanism in LNPs mainly involved π-π stacking forces, and functional groups were not changed. The PVA/LNPs nanocomposite films were fabricated, and their structural and functional behavior were analyzed. The results demonstrated that LNPs were uniformly distributed in the nanocomposite films and formed strong hydrogen bonding interactions with PVA , which improved the thermal stability, mechanical properties, and hydrophobic properties of the nanocomposite films. Notably, LNPs impart the films with excellent UV shielding properties, outstanding antioxidant efficacy, and effective antibacterial activity against S. aureus and E. coli , which makes PVA/LNPs nanocomposite films a potential option for active food packaging.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Meifang Cao,Yuqiao Ma,Tao Ruan,Lifeng Li,Bo Chen,Xueqing Qiu,Di Fan,Xinping Ouyang
The cleavage of C-O bonds in lignin depolymerization was made great progress, but the cleavage of C-C bonds still face challenges. An atomically dispersed Pt loading of 3.30 wt% catalyst, Pt/Nb 2 WO 8 , was prepared by the pyrolysis of ammonium niobate oxalate and sodium tungstate dihydrate with ammonium carbonate as the template. It is found that the decomposition of ammonium carbonate and the doping of W species promoted the orderly growth of niobium tungsten oxide crystals with oxygen vacancy and the formation of a regular porous structure, which was conducive to the dispersion of Pt particles. Pt/Nb 2 WO 8 efficiently cleaved β-O-4, β-1, α-1 and 5–5 bonds. The yield of aromatic monomers for lignin depolymerization reached as high as 49.08% over Pt/Nb 2 WO 8 . Experiments combined with density functional theory calculations revealed that the excellent activity of the Pt/Nb 2 WO 8 catalyst was attributed to the cooperation of atomically dispersed Pt sites and support near the interface. The atomically dispersed Pt species enhanced the dissociation of H 2 , and the Nb 2 WO 8 support with abundant B acid sites provided by W doping and oxygen vacancies activated C-O and C-C bonds of lignin in the reaction. The homogeneous cleavage of C-C bonds dominated the deconstruction of β-1, α-1 and 5–5 bonds. This methodology opens up a facile strategy for the design of atomically dispersed Pt/Nb 2 WO 8 catalyst with higher Pt loading and excellent catalytic activity to the cleavage of both C-O and C-C bonds in lignin.
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ACS Omega
·
2024
·
IF 3.7
Yuanyuan Li,Dongjie Yang,Sijia Wang,Huifang Xu,PengWei Li
To develop reversible pH-responsive emulsifiers of natural origin, alkali lignin (AL) was used to develop oil-in-water Pickering emulsions. AL was first modified to synthesize quaternized alkali lignin (QAL), which displayed pH-responsive properties and demonstrated solubility in both acidic and alkaline solutions. In contrast, QAL exhibited insolubility and formed particles in neutral solutions, thereby making it a suitable candidate for utilization as an emulsifier in doubly pH-responsive Pickering emulsions. At pH 5–9, the emulsions were stable. Above or below this pH range, the system demulsifies, resulting in a reversible Pickering emulsifier with two pH-controlled transitions. On the basis of this pH-dependent behavior, lignin-based Pickering emulsions (LPE) could be subjected to several cycles of emulsification–demulsification by alternating the pH of the aqueous phase between basic and acidic, while the droplet size and storage stability were maintained. Curcumin was used as a drug model to study the loading/release behavior of LPE, finding that 50.08% of curcumin could be encapsulated in LPE. The in vitro release of curcumin was pH-dependent. In addition, LPE exhibited an outstanding protective effect against the ultraviolet-induced degradation of curcumin.
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Green Chemical Engineering
·
2025
·
IF 7.6
Ruan Tao,Zhao Lisha,Ouyang Xinping,Li Lifeng,Zhang Wenwei,Qiu Xueqing
The depolymerization of lignin into aromatic monomers with high yield is the bottleneck of high valued utilization of lignin. In this work, a highly dispersed Pd supported on WO 2.72 (Pd/WO 2.72 ) catalyst was prepared for efficient hydrogenolysis lignin. The highly dispersed Pd, high specific surface area, high content of acidic sites, and hydrogen spillover of Pd/WO 2.72 improved the depolymerization efficiency of lignin. In addition, the depolymerized products were alkylated with the reaction solvent to prevent monomers from re-polymerizing, thus further enhancing aromatic monomers yield. Under 320 º C, 6 h, Bio-oil and aromatic monomers yield reached 77.67% and 28.80%, respectively. Among the aromatic monomers, the tert -butyl group substituted products accounted for 65.71%, of which 77.1% were methoxy-free phenols. It was found that the bio-oil had a calorific value of 38.13 MJ/kg and an IC 50 value of 43 mg/L, showing their potential applications as fuels or antioxidant additives.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
·
IF 5.8
Kai Wu,Bingbing Luo,Qi Cao,Ke Yang,Siyu Wang,Huiyan Zhang
The selective hydrodeoxygenation of lignin-derived compounds is an effective pathway for producing liquid fuels. Here, a series of Co-based catalysts were prepared for converting lignin-derived phenols into alkane fuels. The effects of cobalt loading, Si/Al ratio, reaction temperature, time, and pressure on the distributions of alkane fuels were systematically investigated. The experimental results demonstrated that the in-situ grown LDH structure in Co/HZ-HT significantly improved the pore structure of the catalyst, not only enhancing the dispersion of the metallic particles and overall stability but also strengthening the interaction between the metal and the support. The complete conversion of guaiacol was achieved, and the selectivity of cyclohexane reached 97.5% under the conditions of 200 °C, 2 h, 3 MPa H 2 , and Si/Al ratio of 25. Co/HZ-HT exhibits excellent hydrogenolysis performance and wide applicability, outperforming Co/HZ catalysts prepared using conventional impregnation methods. By extending the feedstock to lignin-derived compounds, the complete deoxygenation of the components and hydrogenation of the aromatic rings were both realized with minimal side reactions.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Daobin Tang,Xuebin Lin,Qi Zhang,Zhenni Wang,Yuhang Liu,Yanqiao Jin,Xinru Wu,Cejun Hu,Pei Yuan
Lignin is continuously investigated by various techniques for valorization due to its high content of oxygen-containing functional groups. Catalytic systems employing hydrolysis‑hydrogenolysis, leveraging the synergistic effect of redox metal sites and acid sites, exhibit efficient degradation of lignin. The predominance of either hydrolysis or hydrogenolysis reactions hinges upon the relative activity of acid and metal sites, as well as the intensity of the reductive atmosphere. In this study, the Pd-MoO x /TiO 2 catalyst was found to primarily catalyze hydrolysis in the lignin depolymerization process, attributed to the abundance of moderate acidic sites on Pd and the redox-assisted catalysis of MoO x under inert conditions. After subjecting the reaction to 240 °C for 30 h, a yield of 48.22 wt% of total phenolic monomers , with 5.90 wt% consisting of diphenols, was achieved. Investigation into the conversion of 4-propylguaiacol (4-PG), a major depolymerized monomer of corncob lignin, revealed the production of ketone intermediates, a phenomenon closely linked to the unique properties of MoO x . Dehydrogenation of the propyl is a key step in initiating the reaction, and 4-PG could be almost completely transformed, accompanied by an over 97 % of 4-propylcatechol selectivity. This distinctive system lays a new theoretical groundwork for the eco-friendly valorization of lignin.
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JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Zhangjun Huang,Ziqi Tang,Hong Tian,Linli Shang,Xuan Huang,Lei Liu,Yanni Xuan
s: Nitrogen-containing compounds become a bottleneck in the conversion of biomass pyrolysis oil into high-value chemicals and fuels, and they are easily oxidized to nitrogen oxides in the subsequent utilization process, causing serious pollution to the environment. Lignin, a biomass component, has an important influence on nitrogen migration during biomass pyrolysis. In this study, we investigated the interaction of lignin model compounds (vanillin and Syringol) with nitrogen-containing components (phenylalanine) during lignin/amino acid co-pyrolysis using tube furnace experiments, thermogravimetric infrared (TG-FTIR) experiments, and gas chromatography-mass spectrometry (Py-GC/MS), as well as the effect of lignin on the pyrolysis gas release and pyrolysis products of phenylalanine, in conjunction with quantum chemical calculation The effect of lignin on the pyrolysis of phenylalanine to styrene was explored. The experimental results showed that during the co-pyrolysis process, lignin modulators (vanillin and Syringol) dramatically reduced the temperature of the first stage of phenylalanine pyrolysis; promoted the pyrolysis oil generation and inhibited the pyrolysis gas generation; vanillin and Syringol promoted the fracture of oxygen-containing and nitrogen-containing functional groups of the side chain of phenylalanine, which resulted in a significant increase in the yields of aromatic hydrocarbons in the pyrolysis oils, with an increase of 32.07 % and 23.41 %, respectively. The simulation results showed that the hydrogen radicals generated by lignin modulators would promote the carbon ring breakage, decarboxylation and intermolecular ring-forming reaction of phenylalanine side chain to generate 1,2-diphenylethene, styrene and NH 3 , and promote the nitrogen-containing carbon chain to undergo intramolecular hydrogen transfer to form HCN, which was converted into styrene pathway showing strong competitiveness.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yan Wang,Kangqi Cao,Wenlong Sun,Xiangxi Lin,Jianwei Wang,Jessica Villarreal,Longzhi Li
Microwave catalytic pyrolysis of lignin is one of emerging technologies for efficiently converting lignin into fuels and chemicals. Molecular sieves (HZSM-5) are widely used as carriers to load metallic components for biomass pyrolysis but often encounter challenges such as high diffusion resistance and insufficient acidity of acidic sites. Traditionally, HZSM-5 is directly modified to enhance the activity of the acidic sites, but this modification is ineffective in improving the metallic components’ activity. Instead, we made nitrogen doping on Fe and then supported on HZSM-5 to construct Fe-N 25 /HZSM-5 catalysts for microwave catalytic pyrolysis of lignin. The N-doped Fe has the effect of “killing two birds with one stone” on enhancing the catalytic activity. The characterization results indicated that N replaced C of the graphitic carbon network to form carbon nitride structure, and further combined with Fe to generate Fe-N bonds, improving the electronegativity of the metallic component. Besides, the loading of N-doped Fe increased the acidity of the catalyst. The utilization of 1.00Fe-N 25 /HZSM-5 obtained the greatest bio-gas yield (35.2 wt%), a hydrogen yield of 27.8 mL/min, bio-oil yield (36.4 wt%) and phenol selectivity of 46.2 %. The likely pathway of microwave catalytic pyrolysis on Fe-N 25 /HZSM-5 was proposed through DFT calculation, using guaiacol as a model compound. The results suggested that N-doped Fe on HZSM-5 8 T tended to break the side-chain methoxy during pyrolysis of guaiacol, with energy barrier of 0.14 eV. This paper provides a promising strategy for modification of microwave pyrolysis catalysts.
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GREEN CHEMISTRY
·
2024
·Vol. 26
·期 5
·2773-2782
·
IF 9.3
Tingting Chu,Xiaoxu Yang,Mingjie Chen,Qing-Shan Shi,Xiaobao Xie,Yanzhu Guo
The conversion of lignin into carbon dots is an emerging technology to make use of this renewable and abundant material. The low yield and low quantum yield of carbon dots from lignin remain key challenges of this technique. Here, prior amino modification of lignin using the Mannich reaction was proposed to improve carbon dot production from lignin by the hydrothermal method. Accordingly, the yield and quantum yield of carbon dots were synchronously improved from 9.8 wt% and 5.36% to 68 wt% and to 42.7%, respectively, because modified lignin suppresses hydrochar formation. A survey of the impact of the lignin structure on carbon dot production, and the structure and property relationship of the as-prepared carbon dots showed that the process could make use of condensed lignin to produce carbon dots with high performance. Techno-economic analysis suggested that this process noticeably reduced the product selling price because of the improved yield. This study provides a strategy to reduce the production cost of carbon dots from lignin, which may inspire the community to extract money out of lignin.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Hongrui Ma,Yutong Yang,Zesheng Xu,Xinru Liu,Fengqiang Wang,Yingjie Qiao,Yongming Song
The severe negative effects of impurities adhering to the external surface of wearable devices can significantly influence the signal transmission, performance, and lifespan of hydrogel sensors. Herein, we developed an ion-conducting hydrogel sensor with a strong adhesive side and a non-adhesive side, similar to a “semi-releasing material.” This hydrogel, formulated using deep eutectic solvents obtained from choline chloride and acrylic acid, contained lignin. This versatile material, exhibiting properties similar to semi-releasing materials, was treated with an AlCl 3 solution on one side. Additionally, the hydrogel was successfully used as a highly adhesive strain sensor for real-time monitoring of various human activity signals. Moreover, the hydrogel demonstrated excellent environmental tolerance and conductivity. Lignin extracted from wood flour endowed the hydrogel sensor with excellent adhesion energy (up to 427.1 J/m 2 ) and UV resistance. Treatment of hydrogels with AlCl 3 completely eliminated their adhesiveness, thereby enhancing fracture elongation and tensile strength. This improvement can be attributed to the absence of carboxyl groups and the formation of a metal-phenolic network. The implementation of this convenient and efficient strategy provides a more feasible approach to address challenges related to impurity adhesion and signal transmission in flexible wearable devices.
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