ACS Applied Materials & Interfaces
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2024
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IF 8.3
Yudong Guo,Xiya Chen,Yuxin Liu,Zhenjun Chen,Peiyuan Guo,Dongxiang Luo,Menglong Zhang,Xiao Liu
In a dual-functional lignin valorization system, a harmonious oxidation and reduction rate is a prerequisite for high photocatalytic performance. Herein, an efficient and facile ligand manipulating strategy to balance the redox reaction process is exploited via decorating the surface of the CdS@ZnxCd1–xS@ZnS gradient-alloyed quantum dots with both inorganic ligands of hexafluorophosphate (PF6–) and organic ligands of mercaptopropionic acid (MPA). Inorganic ion ligands in this system provide a promotion for intermediator reduction reactions. By optimizing the ligand composition on the quantum dot surface, we achieve precise control over the extent of oxidation and reduction, enabling selective modification of reaction products; that is, the conversion rate of 2-phenoxy-1-phenylethanol reached 99%. Surface engineering by regulating the ligand type demonstrates that PF6– and thiocyanate (SCN–) inorganic ion ligands contribute significantly toward electron transfer, while MPA ligands have beneficial effects on the hole-transfer procedure, which is predominantly dependent on their steric hindrance, electrostatic action, and passivation effect. The present study offers insights into the development of efficient quantum dot photocatalysts for dual-functional biomass valorization through ligand design.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Tingting Zhou,Hailin Zhang,Junyou Shi
Lignin, as the largest renewable aromatic resource, has significant opportunities for producing high-value products via catalytic depolymerization. However, its complex structure and stable chemical bonds present challenges to its transformation. This study explores the catalytic depolymerization of lignin to aromatic monomers by means of Dawson-type phosphomolybdovanadate polyoxometalates (POMs), understanding the underlying mechanisms. Furthermore, vanadium modification is employed to adjust the catalyst's oxidative and acidic properties, demonstrating that the vanadium content in Dawson-type POMs greatly influences monomer yield. The highest yield is achieved with H 8 P 2 Mo 16 V 2 O 62 (V2). Optimal conditions include a reaction temperature of 150 °C, 4 h, an oxygen pressure of 1 MPa, a methanol-to-water ratio of 8:2, and a mass ratio of the catalyst to the wood powder being 1:1, which leads to a total yield of aromatic monomers at 24 %. POMs with high REDOX potential selectively oxidizes benzyl hydroxyl groups in lignin to benzyl carbonyl groups under the combined action of acidity and oxidation of polyacids. This weakens the β O 4 bond and promotes C O bond cleavage. This approach, utilizing the tunable oxidative acidity of polyoxometalates to degrade lignin and produce various aromatic monomers, shows promising potential for lignin valorization and advancing a bio-economy based on lignocellulosic resources.
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INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Yan Zhou,Xin Zhou,Songnan Hu,Hanzhi Wu,Junli Ren,Fengxia Yue
As a sustainable alternative for producing materials that can adsorb heavy metal ions (HMI), chemical or physical modification is usually required to improve the activity of lignin. This is because traditional methods of isolating lignin result in a lack of active sites. Herein, we present a simple and efficient method that uses L-cysteine to simultaneously isolate and functionalize lignin from wheat straw, yielding L-cysteine lignin (LCL) with an isolation yield as high as 75 %. Comprehensive characterization revealed LCL retained comparable β-aryl ether bonds to cellulolytic enzymelignin (CEL), representing native lignin with considerable active sites. Additionally, the extraction process introduced amino and carboxylic acid groups to LCL. Compared to CEL, LCL exhibited significantly improved adsorption capacities: 92 mg/g (Cu 2+ ions), 66 mg/g (Pb 2+ ions), 37 mg/g (Cd 2+ ions), and 32 mg/g (Co 2+ ions), respectively. The adsorption kinetics and isotherms trend of Cu 2+ signify the HMI were adsorbed onto LCL through a pseudo-second-order kinetic and Langmuir isotherm adsorption mechanism. LCL also displayed a high surface area (60.03 m 2 /g) on account of the ordered porous structure. XPS and FTIR results confirmed that the L-cysteine (L-cys) substitution in LCL played a crucial role in the adsorption process, indicating that both chemical and physical adsorption contributed to the enhanced adsorption capacity. In summary, this study presents an efficient one-step method for isolating and functionalizing lignin using L-cysteine-assisted extraction. The results demonstrate the promising performance of LCL for adsorbing HMI and contribute to the development of lignin-based adsorption materials.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Chang-An Xu,Xingchi Li,Zhengbang Tong,Zhuangzhuang Chu,Heng Fang,Yang Hu,Xudong Chen,Zhuohong Yang
Although the coating can effectively prevent metal corrosion, it is easy to form micro-pores and micro-cracks during the curing process, and the coating is inevitably damaged by the external environment during use, resulting in a reduction in its protective ability, thereby shortening the service life of the substrate. Inspired by the stress closure function of mimosa, an intelligent anti-corrosion coating with stress closure function against corrosion products (Fe 2+ ) was prepared by using pyridine derivatives and lignin grafted graphene oxide (ATGO). By density functional theory calculation, the binding energy of pyridine group and Fe 2+ was −369.99 kcal/mol, and their strong complexation would facilitate the formation of a dense protective layer at the metal corrosion interface. The test results showed that ATGO-CM coating had high fracture strength (86.9 MPa) and adhesion strength (2.03 MPa), as well as low water vapor permeability (1.3 × 10 -6 g m −1 day −1 Pa −1 ). Electrochemical testing denoted that after soaking in 3.5 wt% saline solution for 100 days, the impedance modulus of the ATGO-CM coating remained at 5.36 × 10 9 Ω·cm 2 at low frequencies (f = 0.01 Hz), which was two orders of magnitude higher than the blank group. Through scratch experiments showed that the complexation effect of pyridine groups and corrosive products could significantly improve the corrosion resistance of the coating, with R ct value of 1.8 × 10 4 Ω cm 2 for the damaged coating, one order of magnitude higher than the blank group. This work not only provided a reference for the preparation of intelligent anti-corrosion coatings with bionic functions, but also increased the added value of biomass materials.
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Journal of Energy Storage
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2024
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IF 8.9
Xuefeng Yu,Dongjie Yang,Jinhao Huang,Qiliang Chen,Weifeng Liu,Fangbao Fu,Xueqing Qiu
Nickel oxide is considered a promising anode material for lithium-ion batteries. Nevertheless, its performance is hindered by significant volume expansion and low electrical conductivity, particularly at larger particle sizes, which lead to a notable decrease in lithium storage capacity and rate performance. To address these challenges, we introduce a nanocomposite strategy to synthesise nickel oxide and lignin-derived porous carbon composites (LPC/Ni/NiO). Through in situ polymerization, lignin macromolecules form a uniform 3D network with nickel carbonate, which, during the subsequent carbonisation process, results in the formation of nickel oxide within a conductive carbon network. This approach reduces the nickel oxide to nanosize and enhances the composite's electrical conductivity, effectively integrating the buffering framework of porous carbon with the high storage capacity of nickel oxide. As a result, the LPC/Ni/NiO composite exhibited significantly improved lithium storage capacity. Notably, when employed as an anode material in lithium-ion half-cells, the optimized composite maintained an excellent specific capacity of 1065 mAh/g after 100 cycles at a current density of 0.2 A/g. It also shown exceptional rate performance, delivering a specific discharge capacity of 505 mAh/g at a current density of 2 A/g, with stable cycling performance. The electrochemical reaction process was further validated using in ex-situ EIS. This study offers valuable insights into scalable synthesis methods for oxide nanocomposites, highlighting their potential as promising anode materials for lithium-ion batteries.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Yi Liu,Shaoyan Wang,Jiarui Liang,Lirong Lu,Yi Xie,Chengrong Qin,Chen Liang,Caoxing Huang,Shuangquan Yao
Demethylation modification of lignin is an effective strategy to overcome the barrier to its high-value conversion. The purpose of this study focuses on the new proton-based ionic liquid (PIL) 1, 2-propanediamine/glycolic acid (PD/GA) as a catalyst and solvent to achieve the targeted oxidation of lignin. The PD/GA solvents have higher selectivity and efficiency. Optimal phenolic hydroxyl (PH)-increment was achieved, demonstrating enhanced demethylating effect on lignin by modulating the acid-base molar ratio, reaction temperature, and reaction time. Compared to ethanolamine/acetic acid (CE/AC) treatment, the PD/GA treatment at molar ratio 1.25, temperature 60 °C, and 3 h increased the PH-content from 37.74 to 59.91 %. Additionally, the lignin treated with PD/GA exhibited excellent recyclability, featuring a larger Brunauer-Emmett-Teller surface area (1.45 m 2 .g −1 ), total pore volume (9.51*10 −3 cm 3 .g −1 ), and mesoporous size (26.15 nm). The treated lignin yielded maximum ultraviolet resistance and antioxidant activity. These results present new avenues for the development of green and efficient lignin demethylation methods.
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JOURNAL OF MOLECULAR LIQUIDS
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2018
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IF 4.513
Jiangdong Dai,Atian Xie,Ruilong Zhang,Wenna Ge,Zhongshuai Chang,Sujun Tian,Chunxiang Li,Yongsheng Yan
In order to efficiently remove sulfamethazine (SMZ) antibiotic from wastewater, in this work, we first described a facile and scalable synthesis of hierarchical porous carbon using industrial by-product sodium lignosulfonate (SLS) as raw source and potassium hydroxide as inorganic template and chemical activator, by a self-templating and in-situ activation method. The Lignin-derived hierarchical porous carbon obtained at an optimal mass ratio of SLS and alkali of 1:3 (LHPC-3) exhibited a largest specific surface area of 2235 m 2 g −1 and pore volume of 1.512 cm 3 g −1 . LHPC-3 possessed a very high saturated monolayer adsorption capacity of 854.7 mg g −1 at 288 K. The pseudo-second-order rate model described the adsorption kinetics data. It was found that this carbon could be also effective in the high salt environment. Physical adsorption played in an important role in the process of capture SMZ molecules from water. This hierarchical porous carbon had good stability and regeneration property, providing the possibility for the practice application. We gave a novel, simple and effective technique to obtain high-performance hierarchical porous carbon for various use, especially for wastewater treatment.
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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
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2024
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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
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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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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Qi Ye,Fei Ge,Xiaohui Yang,Minghao Zhou
The catalytic oxidative depolymerization of lignin and its dimers is key for the effective utilization of biomass. In this work, a metal–organic framework (MOF) was chosen as the precursor, and a series of nickel–manganese bimetallic catalysts with different metal ratios were prepared via a hydrothermal method using 1,3,5-tricarboxylic acid as the ligand. The effects of metal ratio and calcination temperature on the activity of the catalyst were considered, and the oxidative depolymerization of the lignin dimer (2-phenoxy-1-acetophenone) was investigated in detail. The selective conversion of 2-phenoxy-1-acetophenone was achieved over the Ni2Mn1-MOF catalyst in an oxygen atmosphere with methanol as the solvent. Through the optimization of different reaction parameters, including reaction temperature, oxygen pressure, reaction time and solvent, it was found that under optimal reaction conditions (140 °C, 4 h, 0.5 MPa O2), the Ni2Mn1-MOF catalyst exhibited a good catalytic performance for the efficient conversion of 2-phenoxy-1-acetophenone to phenol and methyl benzoate. Furthermore, its specific reaction mechanism was discussed based on the distribution of products in the lignin dimer oxidation process, which was useful for understanding the further oxidative depolymerization of lignin.
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Small
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2024
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IF 13
Xu Han,Qifan Wang,Jiaying Wu,Yuqing Qiao,Yue Kong,Yuhang Lou,Yanqing Gao,Shibin Shang,Zhanqian Song,Jian Li
To address the issue of low pesticide utilization owing to poor dispersibility, low leaf surface adhesion, and poor transport within plants, this study exploits electrostatic interactions between sodium lignosulfonate (SL) and dodecyltrimethylammonium chloride (DTAC) to induce self-assembly, followed by iron ion (Fe 3+ ) chelation and loading with a natural product–based pesticide, rosin–based triazole derivative (RTD), yielding RTD@SL–DTAC–Fe nanomicrocapsules (NMs). It is worth noting that the presence of Fe 3+ enhances the dispersibility of the NMs. The water dispersibility and photostability of RTD are significantly improved after encapsulation, and a stimulus response to laccase is achieved. Leaf-washing experiments confirm the enhanced adhesion of RTD@SL–DTAC–Fe NMs to the surface of rice plant leaves compared to that of free RTD. Fluorescently labeled NMs exhibit bidirectional transport within rice plants, and RTD@SL–DTAC–Fe NMs demonstrates better transport performance than RTD. In vitro and in vivo antifungal tests indicate that encapsulation by NMs significantly enhanced pesticide activity. Field trials demonstrate that NMs exhibited prolonged efficacy compared to RTD. Finally, the safety evaluation confirms the environmental friendliness of the NMs. This study provides valuable insight for optimizing and improving the utilization efficiency and biosafety of natural product–based pesticides.
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危险品化学品经营许可证（带存储）