SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Boqiang Gao,Haoge Liang,Jie Wang,Yan Huang,Jingzhen Wang,Jia Song,Pan Hu,Hu Yang,Shuanglong Ma
Hydroxychloroquine (HCQ) as an antiviral pharmaceutical has been widely detected in the aquatic environment. Adsorption is an effective method for removal of HCQ, but the quantitative study of the adsorption interactions is unclear. In this study, a carboxylated lignin-based sponge (PLC) was fabricated, and the adsorption contributions of electrostatic attraction (EA), hydrogen bond (HB), and π-π electron donor–acceptor (π-π EDA) interactions were quantitatively investigated. The results showed that PLC exhibited excellent adsorption performance under wide pH range (4.0 < pH < 11.0), with the highest adsorption capacity of 0.165 mmol/g. Inhibitor and molecular probe experiments showed that EA and HB were the main contributors to adsorption at neutral and basic pH ranges, respectively. A linear correlation model of the carboxyl groups of lignin-based sponges with the adsorption capacity of EA, HB, and π-π EDA interactions of HCQ ( R 2 > 0.822) and three molecular probes ( R 2 > 0.749) was established, respectively. The optimal adsorption capacity was achieved by the synergistic combination of the deprotonated carboxyl of PLC with the HB of Ka1 amino, EA of Ka2 amino, and the π-π EDA of the quinoline ring. This study provided a new strategy for the quantitative construction of structure–activity relationships of adsorbents.
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CHEMPHYSCHEM
·
2024
·
IF 2.3
Tao Yin,Yang Luo,Arvind Singh Chauhan,Riyang Shu,Zhipeng Tian,Chao Wang,Ying Chen,Navneet Kumar Gupta
In the catalytic transformation of bio-oil into liquid fuels having alkanes via hydrodeoxygenation (HDO), the acid and metal sites in the catalyst are pivotal for promoting the HDO of lignin-derived phenolic compounds. This study introduces a novel bifunctional catalyst comprising phosphomolybdenum-vanadium heteropolyacids (H4PMo11VO40) coupled with Ni/C. The HDO reaction of the model compound guaiacol was carried out under reaction conditions of 230 °C, revealing the superior performance of H4PMo11VO40 with Ni/C catalysts compared to the conventional acids, even at low dosage. The Keggin structure of H4PMo11VO40 provided a solid catalyst with strong acidic and redox properties, alongside advantages such as ease of synthesis, cost-effectiveness, and tunable acid and redox properties at the molecular level. Characterization of Ni/C and the prepared acid demonstrated favorable pore structure with a mesopore volume of 0.281 cm3/g and an average pore size of 3.404 nm, facilitating uniform distribution and catalytic activity of Ni-metal. Incorporating acid enhances the acidic sites, fostering synergistic interactions between metal and acidic sites within the catalyst, thereby significantly enhancing HDO performance. Guaiacol conversion at 230 °C reached 100%, with a cyclohexane selectivity of 89.3%. This study presents a promising pathway for converting lignin-derived phenolic compounds.
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GREEN CHEMISTRY
·
2024
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IF 9.3
Shan Jiang,Riyang Shu,Anqi Wang,Zhuoli Deng,Yuhong Xiao,Jiajin Li,Qingwei Meng,Qian Zhang
High-quality liquid biofuels can be produced from renewable lignin-derived phenolic compounds through the efficient hydrodeoxygenation (HDO) process, in which the traditional catalysts usually include metal site and acid site that catalyzes hydrogenation and deoxygenation procedures respectively. This work presented a novel acid-free NixMoyN/C catalyst from the perspective of green chemistry, providing a new pathway for HDO of lignin-derived phenolic compounds that involves hydrogenation, deoxygenation and hydrogenolysis at the same time. A series of NixMoyN/C catalysts were prepared by varying Ni and Mo molar ratio, where the Ni1Mo3N/C catalyst showed the best HDO performance. Guaiacol was completely converted at 260 °C after 4 h, with 95.8% cyclohexane selectivity. And a small amount of benzene can be obtained as a valuable fuel additive by-product by altering the conventional HDO reaction path. By shortening the reaction time, benzene can be obtained as the intermediate products with a relative high selectivity. Based on the characterizations of XRD, BET, SEM, TEM, XPS, H2-TPD and EPR, the results demonstrate that the multiple active components of Ni1Mo3N/C catalyst allow it to efficiently catalyze the hydrogen activation and C-O bond cleavage even under acid-free condition. The existence of the active phase of Ni, Ni2Mo3N and β-Mo2C, as well as the interaction between Ni and Mo metals, contributes together to achieve an efficient HDO performance. Not only for the various phenolic model compounds, the feasibility of Ni1Mo3N/C catalysts for upgrading raw lignin-oil was also demonstrated, with the hydrocarbon content increasing from 5.7% to 88.4%. Notably, arenes account for 18.2% in the hydrocarbon products, which confirms the occurrence of hydrogenolysis in the catalytic process. This work provides a novel route for the conversion of lignin-derived phenolic compounds to the production of high-quality hydrocarbon liquid biofuels, especially the direct production of arene component.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Yushuai Sang,Mingze Yang,Hong Chen,Yongdan Li
Catalytic lignin solvolysis (CLS) holds promise for efficient lignin utilization, yielding small molecules with minimal or no char formation. However, the role of different active sites of catalyst in CLS are rarely discussed. Here, Ni catalysts on different supports, i.e., SiO 2 , Al 2 O 3 , MgO, and ZrO 2 , were prepared with the aim of manipulating the relative importance of metal and acid-base functionalities to investigate the role of different active sites in the enzymatic hydrolysis of lignin (EHL) ethanolysis. The main ether linkage, i.e., β-O-4, in EHL is cleaved without the participation of a catalyst. Metal sites suppress repolymerization through hydrogenating active intermediates, while acid and base sites facilitate the conversion of phenolic monomers into complex alkylated and etherified products and also promote repolymerization reactions. Among the catalysts, Ni/SiO 2 demonstrated the highest hydrogenation activity and yielded the most monomers (24.7 wt %) at 280 °C for 6 h under 2 MPa H 2 in ethanol. These findings shed light on the catalytic mechanisms in CLS, offering valuable insights for future catalyst design.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Junhao Cui,Zhiyang Zhao,Yongqi Ren,Bailong Chen,Chase Rheinlander,Antonio Xavier Moore,Longzhi Li
Microwave-assisted hydrogenolysis of lignin is an emerging alternative to conventional depolymerization capable of converting lignin into aromatic compounds. Activated carbon (AC) supported Fe component have been shown to be cost-effective for this process, but its cycle stability needs to be improved due to Fe agglomeration. Herein, a strategy of nitrogen doping to promote stability was developed, which utilized melamine (C 3 H 6 N 6 ) as nitrogen source to prepare the catalyst of N-doped AC supported Fe (Fe/N-AC). The catalyst characterization indicated that the N-doped AC acted as anchor points for Fe components, avoiding catalyst deactivation from the source. Fe/N-AC presented an excellent cycle stability, remaining a phenolic compound selectivity of 93.3 % after five cycles and a decrease of only 4.79 % (compared to the first). The DFT calculation results revealed that Fe/N-AC tended to break C Ar -OCH 3 during the hydrogenolysis of guaiacol, with an energy barrier of 0.877 eV. This work proposes a simple and effective strategy to improve the stability of lignin hydrogenolysis catalysts, providing important references for the high-valued utilization of lignin.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yishuai Fu,Wenliang Wang,Hui Miao,Yangyi Cui,Yutong Chen,Ziwei Wang,Guowei Xiao,Bailiang Xue,Weikun Jiang
Obtaining key platform chemicals from lignin is a sustainable refining concept of the non-petroleum route. Rapid pyrolysis is a potential refining technology, and microwave-assisted catalytic depolymerization with low energy consumption is preferred. Herein, we reported the strategy of microwave-initiated depolymerization using a self-designed dynamic vapor flow reaction system with a facilely prepared CMF@Co-MoS 2 -0.18 catalyst, achieving efficient conversion of lignin (Dealkalize) to monophenol. Under constant microwave irradiation (2.45 GHz), the CMF@Co-MoS 2 -0.18 catalyst had excellent dielectric properties (Dielectric loss factor: 0.56) and microwave heating properties (∼140 s rise to ∼ 600℃). Therefore, microwave-initiated depolymerization of lignin showed that the CMF@Co-MoS 2 -0.18 catalyst can improve the monophenol content (54.72 %) and phenol selectivity (35.84 %) under the synergistic effect of microwave absorptivity and catalysis. The reaction of the lignin model and kinetics analysis show that the CMF@Co-MoS 2 -0.18 catalyst increases the yield of monophenol by reducing depolymerization activation energy and selectively breaking the β -O-4 bond. The finite element analysis pointed out that under microwave irradiation, CMF@Co-MoS 2 -0.18 continuously conducted heat to lignin and the lignin vapor would have sufficient energy to collide with the catalyst active site at a high frequency, which led to an increase in the pre-exponential factor and initiated catalytic depolymerization lignin. In summary, we provide a potential pathway for the rapid conversion of lignin into key platform chemicals.
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INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Zhengwen Li,Liheng Chen,Xueqing Qiu
Lignin, a natural macromolecule renowned for its exceptional UV-blocking capabilities, has gained attention as a promising material for encapsulating chemical sunscreens. However, the inherent heterogeneity and dark coloration of lignin have limited its application in the sunscreen industry. This study presents a novel approach to obtaining uniform and light-colored lignin through fractionation of alkali lignin using a green co-solvent system of dimethyl carbonate and ethanol. The processed lignin was then utilized to create regular-shaped microspheres via the emulsion solvent evaporation (ESE) method. By optimizing the preparation conditions, the chemical sunscreen avobenzone (AVO) was successfully encapsulated within these lignin microspheres, achieving an AVO loading capacity of up to 70 %. The resulting lignin microsphere-coated avobenzone (LM/AVO) microcapsules demonstrated broad-spectrum UV resistance and sustained photostability for up to 12 hours under continuous UV exposure. Additionally, the microcapsules exhibited robust antioxidant properties and negligible skin penetration, highlighting their excellent safety profile. These findings indicate the significant potential of lignin-based microcapsules for innovative and effective sunscreen formulations.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Sheng Dai,Xueyan Zang,Xuehan Zhang,Meiduo Ren,Hua Qiu,Kunlin Chen
The increasing emphasis on green and sustainable development has propelled the integration of lignin into polymer matrices as a promising trend. Lignin, a highly reactive biomass material endowed with hydrophilic functional groups, presents significant potential in polymer applications. However, its intrinsic dark coloration poses a considerable challenge to its polyurethanes (PU) use. In this study, lignin was chemically modified through sulfonation, introducing an abundance of sulfonic acid groups that not only enhanced its hydrophilicity but also markedly reduced its color intensity. Additionally, 2-methacryloyloxyethyl phosphorylcholine diol (MPC-diol) was employed as a chain extender in conjunction with sulfonated lignin (SL) to further augment the hydrophilicity of the resulting PU. The incorporation of both anionic and cationic species within the polymer side chains facilitated improved polymer chain interactions. The synergistic combination of polycaprolactone (PCL) soft segments and SL end-capped segments enabled the formation of multiple hydrogen bonds and disulfide linkages, culminating in waterborne polyurethanes (WPU) characterized by superior mechanical properties and self-healing capabilities. The application of these light-colored, SL-based polycarbonate waterborne polyurethane (PCPUSL) coatings to fabrics significantly enhanced their biocompatibility and antimicrobial properties. This development represents a green, sustainable, and highly flexible WPU coating with exceptional self-healing properties and promising potential for diverse applications.
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Small
·
2025
·Vol. 21
·期 8
·2409803
·
IF 12.1
Jianfeng Ma,Shumin Zhang,Xin Shi,Linxin Dai,Zhenzhen Liu,Xinge Liu,Xihong Lu,Zehui Jiang
A nitrogen-coordinated Fe single-atom catalyst (SA Fe-N/C) is synthesized using a homogeneous ethanol-based dissolution system with bamboo kraft lignin serving as the carbon source. Uniformly dispersed Fe atoms with an interatomic distance of less than 2 Å throughout the SA Fe-N/C structure are revealed through X-ray absorption spectral analysis and HAADF-STEM images, which possessed a high Fe loading of 2.69%. The degradation rate of bisphenol A (BPA) approached 99% within 5 min, with the observed rate constant ( k obs ) of the catalysts markedly increasing from 0.070 to 0.615 min −1 . The catalyst-mediated electron transfer pathway is identified as the predominant mechanism for BPA degradation. Both experimental data and DFT analysis of the nitrogen ligands demonstrated that pyridinic N-coordinated Fe single atoms are the principal active sites, attributed to the enhanced electron density and delocalization concentrated around the Fe sites. These findings significantly elucidate the role of nitrogen ligands in designing efficient lignin-derived carbon single-atom catalysts for environmental applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Xuan Li,Yixin Yun,Yitong Wang,Wanbin Zhu,Quan Bu,Yaxun Fan,Hongliang Wang
Inexpensive biomass materials hold great potential for the development of green delivery systems aimed at improving the extremely low utilization efficiency of pesticides. However, current systems face challenges in achieving both high encapsulation rates and drug loading capacities. This study introduces a novel method using chitosan (CS) and sodium lignosulfonate (SL) to co-assemble with avermectin (AVM), a widely used hydrophobic pesticide, forming AVM-CS-SL micro-nano capsules. Engineered under optimized conditions of pH 5 and 40 °C, the capsules exhibit an AVM encapsulation efficiency of 84.27 % and a loading capacity of 90 %. The AVM-CS-SL capsules demonstrate multifunctional attributes that enhance pesticide application. The capsules, with an average diameter of 356 nm, facilitate stable embedding in leaf grooves and enable effective adhesion to leaf surfaces, thereby improving their resistance to wash-off by rain compared to conventional formulations. Their core-shell structure protects AVM from photodegradation, ensuring long-term stability and efficacy. The capsules also exhibit enhanced bioactivity, with higher mortality rates in Plutella xylostella larvae and low genotoxicity to Vicia faba plants. These findings highlight the strategy of developing multifunctional delivery systems by the co-assembled carrier materials with active ingredients, offering an effective solution for the sustainable development of society and environment.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Xinyi Xie,Lifeng Li,Xiangyu Wang,Qiyu Liu,Xinping Ouyang,Xueqing Qiu
Effective fractionation of lignocellulose into hemicellulose, cellulose, and lignin is the precondition for full-component valorization. Generally, harsh reaction conditions are used to improve fractionation efficiency, which leads to severe lignin condensation and inhibits its value-added applications. To address this issue, a novel biphasic system consisting of molten salt hydrates (MSHs) and n-butanol was developed for birch fractionation. After the removal of hemicellulose in dilute acid, the solid residue composed of cellulose and lignin was carried out in biphasic system conversion. Cellulose was selectively converted into 73.3% yield of glucan oligomers and 16.8% glucose in the MSH phase, while lignin was in situ-extracted into the n-butanol phase with a high yield of 98.1%. Mechanism studies revealed that the in situ extraction together with Cα–OH group modification by n-butanol synchronously protected lignin β-O-4 linkages from cleavage, resulting in a high β-O-4 content of 53.7%, indicating that 87.7% of β-O-4 linkages in birch has been preserved. After depolymerization, a promising monophenol yield of 22.4% was obtained, which was 81.5% of the theoretical maximum monophenol yield obtained from birch. This fractionation strategy can also be used in softwood and herbaceous, showing a splendid separation efficiency as well as a high yield of noncondensed lignin production.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Zhe-Hui Zhang,Ming-Jie Song,Saravanakumar Elangovan,Zhuohua Sun,Tong-Qi Yuan
Lignin is the largest renewable source of aromatic building blocks in nature and has great potential as a starting material for the production of bulk or functionalized aromatic compounds, providing a suitable alternative to widely used petroleum-derived chemicals. In this work, we present a novel 1,4-cyclohexanediol (CHDO) preparation from lignocellulose. In contrast to conventional methods, this pathway has taken the lignin-degrading monomers as a starting point, and flexibly employs a series of oxidative and catalytic reactions to achieve the preparation of CHDO. The proposed pathway consists of a two-step chemical process to efficiently obtain high yields of CHDO from lignocellulose. The first step is the oxidation of lignin-derived monophenols to p -hydroxyl phenolic compounds using the Dakin oxidation reaction (yield>80%), and finally the de-functionalization and hydrogenation of the resulting monomers using the hydrodeoxygenation (HDO) reaction.
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