INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Xin Zhao,He-Fei Wan,Shao-Fei Sun,Ce Gao,Shuang Zhang,Run-Cang Sun
Lignin commonly has a low antioxidant activity despite acting as a natural antioxidant . Most of the reported chemical reagents for enhancing lignin phenolic hydroxyl content contain halogen or metal elements, which is expensive, toxic environment and non-recyclable. Here, a cost-effective and eco-friendly technique for increasing the phenolic group content and antioxidant capability of lignin was described. Protic ionic liquids , an effective demethylating reagent with advantages of zero halogen, low cost and recyclability was applied for lignin demethylation . Quantitative 1 H NMR and semi-quantitative 2D HSQC NMR analyses revealed the conversion of methoxy groups to phenolic groups. Typically, ethanolamine acetate was able to efficiently demethylate the methoxy of raw lignin at a rate as high as 44.73 %, which increased the amount of phenolic group in RL to 215.69 %. Besides, the recovery rate of [HOAc]-based protic ionic liquids and lignin was both over 90 %. The IC 50 value of organic lignin (OL) on scavenging of 2,2-Diphenyl-1-picrylhydrazyl was decreased to 0.15 mg/mL, which was better than natural or synthesized antioxidative chemicals.
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ACS Catalysis
·
2024
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IF 11.3
Haoquan Guo,Jiwu Zhao,Yu Chen,Xinyu Lu,Yue Yang,Chenrong Ding,Lizhi Wu,Li Tan,Jinlin Long,Guohui Yang,Yu Tang,Noritatsu Tsubaki,Xiaoli Gu
Lignin derivatives are one class of attractive alternative feedstocks for the production of renewable biofuels. Herein, hydrodeoxygenation (HDO) of lignin derivatives was carried out using a single-atom catalyst (SAC) comprised of Ni1 SAC on β-Mo2C. A number of lignin-derived compounds have been investigated, and nearly 100% yield of biofuel molecules was converted from various lignin derivatives through the HDO reaction, demonstrating that Ni1/β-Mo2C has remarkable potential for the production biofuels through catalytic hydrodeoxygenation of lignin derivatives. The reaction mechanism of DHE over single-atom catalyst Ni1/β-Mo2C was confirmed based on comprehensive characterizations of catalysts and DFT calculations. Interestingly, the Ni single-atom active sites alter the reaction pathway by shifting the geometry of the adsorbed intermediate from a vertical to horizontal conformation, which lowered the reaction energy barrier and improved the selectivity to biofuel molecules, resulting in extraordinary catalytic activity. This study suggests an avenue for single-atom catalysis in chemical transformations of lignin derivatives into biofuels.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Peng Qiannan,Zhao Cheng,Wang Xiaopeng,Cheng Kelin,Wang Congcong,Xu Xihui,Lin Lu
Lignin, as the abundant carbon polymer, is essential for carbon cycle and biorefinery. Microorganisms interact to form communities for lignin biodegradation, yet it is a challenge to understand such complex interactions. Here, we develop a coastal lignin-degrading bacterial consortium (LD), through “top-down” enrichment. Sequencing and physiological analyses reveal that LD is dominated by the lignin degrader Pluralibacter gergoviae (>98%), with additional rare non-degraders. Interestingly, LD, cultured in lignin-MB medium, significantly enhances cell growth and lignin degradation as compared to P. gergoviae alone, implying a role of additional outliers. Using genome-scale metabolic models, metabolic profiling and culture experiments, modeling of inter-species interactions between P. gergoviae , Vibrio alginolyticus , Aeromonas hydrophila and Shewanella putrefaciens , unravels cross-feeding of amino acids, organic acids and alcohols between the degrader and non-degraders. Furthermore, the sub-population ratio is essential to enforce the synergy. Our study highlights the unrecognized role of outliers in lignin degradation.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 4
·973-979
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IF 4.4
Peidong Ren,Lei Shi,Ziwang Kan,Jiaxiao Bai,Yunyi Liu,Shucheng Yang,Siqi Li,Song Liu
The electrochemical conversion of lignin for the production of high-value aromatic compounds holds immense potential. However, the process of depolymerizing lignin faces significant challenges due to its intricate structure, particularly the existence of C–C bonds, resulting in low conversion and product yields. In this work, we report the successful synthesis of a molecular palladium catalyst and its inaugural application in the electrochemical conversion of lignin model compounds. This catalyst with well-defined coordination structure demonstrates exceptional efficacy and achieves a remarkable 99% conversion rate for the lignin model compound 2-phenoxy-1-phenylethanol with a yield of 32% of the benzaldehyde product while valuable hydrogen is produced at the electrode under ambient conditions. Furthermore, employing radical trapping and EPR test point that the tBuO˙ radical was the key to inducing C–C cleavage for high conversion and enabled a comprehensive elucidation of the possible reaction pathways involving radical/radical cross-coupling. Based on this study, we believe that molecular catalysts will open a new chapter in the electrocatalytic conversion of lignin.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Shihao Feng,Qi Fan,Qin Ouyang,Xilin Zhang,Kun Liang,Qing Huang
Lignin-derived porous carbon (LDPC) is a low-cost and sustainable electrode material for supercapacitors . However, the complex three-dimensional amorphous structure of lignin brings challenges to the morphology and structure control of LDPC, which limits the electrochemical performance of these electrodes. Herein, a series of LDPCs with different particle morphologies and hierarchical pore structures are prepared by spray drying and KOH activation. It is found that the morphology and structure of LDPCs can be effectively controlled by adjusting the spray drying temperature and KOH ratio. A systematic investigation has been conducted on the relationship between the morphology and structure of LDPCs and their electrochemical performance. The preferred LDPC exhibits excellent electrochemical performance, showing high specific capacitances of 372.5 F g − 1 and 264.8 F g −1 at current densities of 0.2 A g −1 and 20 A g −1 , respectively, in the three-electrode test. The symmetric supercapacitor assembled with the LDPC electrode material exhibits superior cycling stability and energy density . After 10000 cycles of continuous charging and discharging at current density of 1 A g −1 , the specific capacitance retention is as high as 96.4%. When the power density is 493.3 W kg −1 , the energy density reaches ∼9.1 Wh kg −1 . This work offers a viable method for regulating the morphology and structure of LDPC electrode material for high-performance supercapacitor application.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Weijie Lin,Han Han,Xilai Yan,Jie Xie,Hongshen He,Shibo Han,Dengwen Ning,Ajoy Kanti Mondal,Shuai Wu,Fang Huang
The preparation of natural polymer-based highly conductive hydrogels with reliable durability for applications in supercapacitors (SCs) is still challenging. Herein, a facile method to prepare alkaline lignin (AL)-based polypyrrole (PPy)-rich, high-conductive PPy@AL/PEGDGE gel was reported, where AL was used as a dopant , polyethylene glycol diglycidyl ether (PEGDGE) as a cross-linking agent, and PPy as a conducting polymer . The PPy@AL/PEGDGE gel electrode materials with hollow structures were prepared by electrochemical deposition and chemical etching method and then assembled into sandwich-shaped SCs. Cyclic voltammetry (CV), galvanotactic charge discharge (GCD), electrochemical impedance spectroscopy (EIS) and cycling stability tests of the PPy@AL/PEGDGE SCs were performed. The results demonstrated that the SCs can achieve a conductivity of 25.9 S·m −1 and a specific capacitance of 175 F·g −1 , which was 127.4 % higher compared to pure PPy (77 F·g −1 ) electrode. The highest energy density and power density for the SCs were obtained at 23.06 Wh·kg −1 and 5376 W·kg −1 , respectively. In addition, the cycling performance was also higher than that of pure PPy assembled SCs (50 %), and the capacitance retention rate can reach 72.3 % after 1000 cycles. The electrode materials are expected to be used as sensor and SCs devices.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Tingting Liu,Yanfan Yang,Li Yan,Biying Lin,Lin Dai,Zhanhua Huang,Chuanling Si
Adhesives are used extensively in the wood industry. As resource and environmental issues become increasingly severe, the development of green and sustainable biomass-based adhesives has attracted increasing attention. In this work, a green wood adhesive is developed from poly(vinyl alcohol) and lignin with molecular designs of lignin extending beyond those in nature. The lignin undergoes extraction from corncob residue, aldehydration, and phenolisation (phenol, resorcinol, and catechol) to significantly increase the phenolic hydroxyl groups (over 7.92 mmol/g), which has the effect of enhancing the hydrogen bonding force between the adhesive and the wood, thereby greatly improving adhesive performance. Compared with pure PVA, polyphenol lignin-containing PVA showed improved adhesion strength and hydrophobicity . PVA/resorcinol-lignin has the significantly improved wood lap shear strength (6.27 MPa, 77.6 % improvement) and hydrophobicity (almost 100 % increase in wet shear strength). This research not only provides a green and high-performance alternative raw material for wood adhesives but also broadens the path for large-scale application of biomass.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
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IF 7.7
Baojie Liu,Huali Zeng,Shuo Wang,Yunbiao Pang,Chengrong Qin,Chen Liang,Caoxing Huang,Shuangquan Yao
High-purity pulp fibers can be obtained by using chlorine dioxide to oxidize lignin. However, organic halogen compounds (AOX) are generated from chlorination side reactions during the lignin oxidation process. In this study, phenolic lignin model compounds with different substituents were selected. The effects of substituent position on the production of free radicals and oxidative ring opening in benzene rings were analyzed. It was found that the structural transformation of lignin and the reaction consumption of ClO 2 were significantly changed under high concentration of ClO 2 . The molar consumption ratio of compound to ClO 2 was increased from 1:2 to 1:3. Quinone , an intermediate product that promotes the formation of phenoxy radicals, was found to be stabilized in the reaction. This is attributed to that the benzene ring of lignin is activated through long-range electrostatic interactions . The formation of free radicals and the oxidative ring-opening reaction of benzene rings were facilitated. The efficient oxidation of lignin by ClO 2 was fulfilled. Chlorination reactions of lignin were suppressed at elevated oxidation efficiency. The pollution load of wastewater was significantly reduced. AOX generation was reduced by 69.27 %. This provides a new method for efficient oxidative degradation of lignin and preparation of high purity pulp fiber.
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JOURNAL OF THE ENERGY INSTITUTE
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2024
·
IF 5.6
Bowen Luo,Xiaoxin Chen,Yongxiang Guo,Riyang Shu,Chao Wang,Jianping Liu,Junyao Wang,Zhipeng Tian,Ying Chen
Hydrodeoxygenation (HDO) is a crucial technique for upgrading biomass-derived compounds, playing a significant role in the advancement of sustainable energy technologies. Under harsh reaction conditions, conventional HDO catalysts often suffer from reduced efficiency due to particle aggregation. This study presents a highly efficient Ni/Al 2 O 3 -C catalyst that mitigates this issue by stabilizing Ni metal particles and enhancing metal-support interactions. Characterization of the catalyst was carried out using XRD, TEM, and CO-TPD, which revealed that the incorporation of Al species improved metal dispersion and reduced the size of the Ni particles. Guaiacol, a phenolic compound derived from lignin, was chosen to evaluate the HDO performance under mild conditions. The optimized Ni/3Al 2 O 3 -5C catalyst achieved a guaiacol conversion of 99.9 % with a cyclohexane selectivity of 99.8 % at 210 °C. The outstanding performance is attributed to the high hydrogenation capacity of the small Ni particles and the acid sites on the carbon surface. Metal-support interactions stabilize the Ni particles, preventing leaching and deactivation. The catalyst has also exhibited comparable effectiveness in the HDO of both lignin-derived compounds and lignin-oils, confirming its adaptability across various substrates. The study demonstrates that Al 2 O 3 -C plays a crucial role in enhancing both the structural stability and catalytic efficiency of HDO catalysts, offering a promising approach for upgrading biomass-derived compounds.
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Journal of Cleaner Production
·
2024
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IF 9.7
Yang Liu,Chunbao Zhou,Asif Ali Siyal,Chenglong Liu,Yingwen Zhang,Jie Fu,Huimin Yun,Jianjun Dai,Xiaotao Bi
In this paper, a cleaner pyrolysis strategy combining microwave heating, catalyst and carbon dioxide was explored for converting biomass components into higher quality products. Catalytic pyrolysis was more favorable for the decomposition and conversion of complex biomass structures. For furfural residue pyrolysis , potassium sulfate contained in sample served as the main catalytic component. Potassium sulfate promoted the increase of phenols in bio-oil. Notably, carbon dioxide atmosphere promoted the decomposition of substances and exerted a significant effect on biomass pyrolysis , which increased bio-oil yield and declined gas yield. When the pyrolysis atmosphere was changed from nitrogen to carbon dioxide, the I D /I G ratio decreased from 1.07 to 0.74, indicating that carbon dioxide decreased defect structure in biochar. Carbon dioxide enriched the porous structure and surface roughness of biochar. Also, carbon dioxide as a carrier gas was found to be more effective than nitrogen in improving the heating values of biochar and the acidity of bio-oil under carbon dioxide was lower than that under nitrogen, which was conducive to the subsequent utilization of biochar and bio-oil. Carbon dioxide promoted the production of alcohols, alkenes , and alkanes in bio-oil. Beneficially, the interaction of cellulose and lignin inhibited the release of hydrogen chloride . At last, this study also provides insights into the mechanism of catalyst and CO 2 on biomass microwave pyrolysis .
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FOOD HYDROCOLLOIDS
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2024
·
IF 11
Jianming Tao,Lin Lei,Fayin Ye,Guohua Zhao
Colloidal lignin particles (CLPs), derived from ubiquitous dietary fiber, are emerging as viable emulsifiers due to their sustainability and biocompatibility. Despite appealing advantages, the emulsifying capacity of CLPs in triglyceride matrices (e.g. edible oil) is constrained by their inadequate amphipathic properties. As characterized by intermediate wettability and renewable provenance, sodium caseinate (Cas) is proposed as a promising surface modifier to enhance the interfacial performance of CLPs. This study conscientiously delved into the adsorption dynamics of Cas onto CLPs and elucidated the ramifications of Cas coating on the physicochemical attributes of CLPs and consequent sunflower oil-loaded emulsions. The presence of non-covalent forces was a crucial factor in consolidating the chemisorption of Cas onto CLPs, where hydrophobic interactions exerted the major contribution. Progressive increments of Cas coating were observed to enhance particle size and hydrophobicity while diminishing the absolute surface charge of the colloidal entities, thus bolstering their interfacial affinity accompanied by distinct adsorption behaviors. As a result, Cas molecules improved the stability of CLPs-based Pickering emulsions mainly by thick interfacial layers and fortified network structures. With the highest level of curcumin retention observed in the 0.16Cas-CLPs emulsion, the encapsulated systems stabilized by modified CLPs effectively protected photosensitive compounds against ultraviolet irradiation.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Hairui Jiao,Guifeng Xu,Yushuai Sang,Hong Chen,Yongdan Li
Herein, we reported a one-pot method that directly converting enzymatic hydrolysis lignin (EHL) into cycloalkane fuels using a Ni catalyst derived from Ni-Al hydrotalcite (NiAl-LDH). The effects of Ni/Al ratio and reduction condition on the catalytic activity have been examined. The catalyst obtained from the reduction of NiAl-LDH at 460 °C (Ni 2 Al 1 -re460) shows the highest activity among the catalyst samples examined, attributed to its abundant Lewis acidic sites, small-sized Ni metal particles, and large specific surface area. At optimized reaction conditions (320 °C, 3 MPa H 2 , 6 h), this catalyst achieves 100% EHL conversion and complete oxygen removal and improves the calorific value of the products from 25.0 MJ kg −1 to 42.5 MJ kg −1 . The detected products are cycloalkane dimers and monomers with their carbon numbers within the range suitable for gasoline and diesel, and other large molecules with uncertain structures also predominantly consist of cycloalkane rings.
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