Science China-Materials
·
2026
·
IF 7.7
Chen Jiayue,Zhou Zhou,Luo Weili,Yue Yiying
Recent advancements in sustainable bio-sourced functional materials have focused on enhancing the valorization of lignin-derived biopolymers through innovative transformation methodologies. This study highlights breakthroughs in lignin-based Z-scheme heterojunction photocatalytic systems, emphasizing extended spectral responsiveness, optimized interfacial photoexcited carrier separation and reduced energy loss mechanisms. Two photocatalysts, Bi 2 WO 6 (BWO) and ZnIn 2 S 4 (ZIS) were co-engineered via a Z-scheme charge-transfer pathway using coaxial electrospinning and hydrothermal synthesis with lignin-based carbon nanofibers (CNFs), preserving the fibrous skeleton intact. The all-component photocatalytic nanomembrane exhibited superior mechanical strength (Young’s modulus = 20.38 MPa, toughness = 2.48 kJ/m 3 ) under wet conditions along with accelerated stabilization kinetics (1°C/min, representing a 10-fold increase), resulting in significant energy savings. Using methylene blue (MB) as a model pollutant, the CNFs@BWO/ZIS nanomembrane achieved 94.4% degradation efficiency ( k = 0.01664 min −1 ) after 120 min of solar irradiation, while maintaining excellent recyclability through five successive cycles. Furthermore, we elucidated the systematic mechanism of surface charge-carrier migration in the Z-scheme heterojunction and MB decomposition. This photocatalytic system utilizing sustainable biomass functional materials paves the way for wastewater treatment, with the goal of achieving peak carbon emissions and carbon neutrality. The alternative text for this image may have been generated using AI.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1748-1754
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IF 5
Shaoyuan Guo,Xinli Tong,Lingwu Meng,Guobao Yang
Selective oxidative C–C and C–O bond cleavage is of significance to the efficient utilization of biomass and biomass-derived platform compounds. In this work, the selective oxidative cleavage of C–C and C–O bonds has been developed with an iron-based catalyst (Fe–N–C) in the presence of molecular oxygen. Specifically, the β-O-4 lignin model compound was successfully converted to phenol and methyl benzoate in a methanol solvent, where the substrate conversion was 95.0% and the yields of phenol and methyl benzoate were 94.9% and 63.7%, respectively, when the reaction was performed with the Fe–N–C-850 catalyst at 120 °C for 4 h. Also, the oxidative transformations of other lignin models to phenols and methyl benzoates were achieved. Further investigations showed that the existence of the Fe3C phase in the catalyst plays an important role in the aerobic oxidative cleavage of C–C and C–O bonds in the β-O-4 lignin model.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 3
·1179-1190
·
IF 9.8
Yaohong Zhou,Wanming Xiong,Yujing Jin,Peng Wang,Weiqi Wei,Jiliang Ma,Xiaohua Zhang
Conversion of lignin feedstocks into aromatic chemicals is a highly desirable target for biorefineries, and their depolymerization often requires high temperatures and harsh conditions. In this work, a process optimization involving several factors, including catalyst dosage, reaction temperature, reaction time, oxygen pressure and solvent effect, towards vanillin production from the oxidation of lignin-based vanillyl alcohol in a base-free solvent over a LaFeO3 perovskite was proposed. The results pronounced that the LaFeO3 perovskite exhibited excellent catalytic performance for affording a 100.0% conversion rate of vanillyl alcohol and 33.0% vanillin yield with the addition of 0.1 g LaFeO3 dosage at 180 °C for 2 h under 1.0 MPa O2 supply in ethyl acetate solvent. Furthermore, the presence of oxygen vacancies (Fe3+–□–Fe2+) in the LaFeO3 perovskite contributed to combining with molecular oxygen to generate the active species [Fe3+O2−], which played a key role in the oxidation of vanillyl alcohol and dominated the formation pathway of vanillin. On the other hand, reusability tests manifested that the performance of LaFeO3 decreased gradually with the increase of consecutive runs and was strongly negatively related to the amount of carbon deposits, as carbon deposits would prevent vanillyl alcohol from being accessible to active sites. Nevertheless, the performance of the spent LaFeO3 catalyst could be easily regenerated by a simple calcination approach. Overall, this work provides the possibility of a scalable strategy for constructing LaFeO3-based perovskites as efficient and reusable catalysts for vanillin production from biorefinery lignin.
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FUEL
·
2022
·
IF 8.035
Zhi Yang,Bowen Luo,Riyang Shu,Zhuojie Zhong,Zhipeng Tian,Chao Wang,Ying Chen
Hydrodeoxygenation (HDO) is an indispensable reaction in the field of fuel and chemical production, and the synergistic effect of metal–acid sites in the catalyst makes great influence to it. Herein, a bifunctional catalyst of Ru/C combined with phosphotungstic acid (HPW) was employed for the hydrodeoxygenation (HDO) of lignin-derived compounds to make full use of the synergistic effect of active metal–acid sites. HPW possessed a temperature-controlled phase-transfer behavior, which made it dispersed well on the surface of Ru/C catalyst and resulted in a close integration of acid site with metal site. Ru/C-HPW catalyst also owned the advantage of high reaction rate and good recyclability, which exhibited no obvious catalytic activity loss after 5 runs. Lignin-derived phenolic compounds including monomers and dimers enabled to obtain an efficient transformation to cycloalkanes at the temperature of 200 °C. Moreover, a high HDO reaction efficiency of raw lignin-oil was also observed in this study, with the increasing hydrocarbon content from 5.5% to 78.9%. This novel catalytic system can achieve a high HDO efficiency under mild conditions.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Jiansu Ran,Ruixue YangCheng,Yuntong Cui,Jianjian Wang
Selective and efficient low-temperature hydrodeoxygenation (HDO) of lignin derivatives in water for the production of valuable biofuel and chemicals is still challenging. Herein, we reported biomass carbon-supported ultrafine Pd nanoparticles as highly active and stable catalysts for low-temperature HDO of vanillin (a typical lignin-derived compound) to 2-methoxy-4-methylphenol (MMP). We found that the abundant carboxyl groups on the resultant catalyst greatly accelerated the conversion of the generated intermediate (vanillyl alcohol, VAL), and then, the synergistic catalysis between carboxyl groups and Pd nanoparticles promoted the efficient production MMP through a free-radical pathway. Other lignin derivatives with different functional groups were also efficiently converted to the corresponding products over the prepared catalyst. This work may provide a new idea for designing a biomass-derived catalyst for efficient transformation of various lignin derivatives to produce value-added biofuels and chemicals.
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Journal of Energy Storage
·
2022
·
IF 8.907
Rongbiao Shen,Peng Lian,Yan Cao,Ying Chen,Li Zhang,Xinxin Sheng
To promote the high-value utilization of lignin, a novel, all lignin-based chemically crosslinked sponge (CCL) was prepared and used to encapsulate phase change materials (PCMs) to solve problems associated with PCM leakage in practical application. In a straightforward, one step vacuum impregnation method, myristyl alcohol (MA), n-docosane (C22), and polyethylene glycol (PEG) phase change materials were encapsulated in the CCL sponges that were used as supporting material to prepare CCLPCMs, which were named as MA/CCL, C22/CCL, and PEG/CCL, respectively. Benefiting from the strong capillary action provided by the unique 3D continuous porous structure of the CCL, the mass loading of PCMs in the corresponding CCLPCMs are reached up to 93.1 ± 1.5 %, 90.2 ± 1.2 %, and 91.2 ± 0.6 %, respectively. It is also worth noting that η values of the corresponding CCLPCMs reached 99.4 ± 0.9 %, 100.9 ± 1.0 %, and 99.7 ± 1.0 %. The CCLPCMs showed excellent encapsulation capabilities, thermal reliability after 300 heating and cooling cycles and high solar-to-heat conversion capability over 30 cycles. These results provide a fresh, green, sustainable, and promising strategy to promote high-value utilization of lignin and design shape stability PCMs for heat energy storage.
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Green Energy & Environment
·
2022
·
IF 12.781
Yang Zhou,Qiang Zeng,Hongyan He,Kejia Wu,Fuqiao Liu,Xuehui Li
In order to better understand the specific substituent effects on the electrochemical oxidation process of β -O-4 bond, a series of methoxyphenyl type β -O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para -methoxy (on the aryl ring closing to C α ) and C α -OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the C α -C β bond cleavage induced by electrochemical oxidations.
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POLYMER COMPOSITES
·
2022
·Vol. 43
·期 11
·7871-7881
·
IF 3.531
Dongdong Zeng,Yuhang Su,Jiaqi Dong,Xiaojun Ma,Lili Yu,Youjun Lv
In this study, four typical biocomposites from lignin blended with poly-3-hydroxybutyrate-3-hydroxyhexanoate (PHBH) using inorganic nanoparticles (INPs) (SiO 2 , MMT, CaCO 3 , and BN) as fillers were evaluated, which enhanced the thermal, mechanical, and barrier properties of composites. The results revealed that the selection of suitable INPs doped into the lignin/PHBH (L/P) composites was an important approach to achieve available function. MMT/L/P nanocomposites were significantly higher than those of untreated L/P composites in thermal stability (T max exceed 10%) and barrier properties (water vapor and oxygen resistance increased by 48% and 46%), and BN particles increased the initial thermal decomposition temperature by 8%. The elongation at break of CaCO 3 /L/P and BN/L/P composites were increased by 344% and 319%, while SiO 2 /L/P composites had the best tensile strength (18.8 MPa). Besides, the INPs/L/P nanocomposites in this paper exhibited excellent ultraviolet (UV) resistance and might become potential anti-UV packaging materials for grease foods.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Fangbao Fu,Dongjie Yang,Yukang Fan,Xueqing Qiu,Jinhao Huang,Zhixian Li,Wenli Zhang
Nitrogen-doped porous carbons have emerged as promising electrode materials for supercapacitors. However, the precise control of carbon geometry and the effective doping method remain challenging. Herein, a confined self-assembly template and in-situ mild activation strategy is proposed to prepare cubic lignin composite precursor, followed by co-pyrolysis with melamine at a high temperature for nitrogen-doped hierarchical porous carbons (N-HPLCs). The zinc oxalate template has the coupling effect of confinement and mild activation during carbonization, which not only prevents the restacking of the carbon matrix but also generates zinc cyanamide intermediate to avoid excessive loss of nitrogen species. The optimized N-HPLCs exhibit an accordion-like framework with interconnected porous sheets, ultrahigh edge-nitrogen doping level (up to 12.20 at.%), and a total nitrogen doping level of 14.09 at.%. Consequently, it shows a high gravimetric capacitance of 354 F/g at 0.2 A/g, an extraordinary surface-area-normalized capacitance of 82.1 ± 0.2 μF/cm 2 , and good rate capability in supercapacitor applications. Moreover, the fabricated coin-type symmetric supercapacitor displays a high energy density of 12.9 Wh/kg at 161.9 W/kg and superior cycling stability with a 99.5% capacitance retention after 16,000 cycles at 2.0 A/g. This work offers a novel method for preparing nitrogen-enriched lignin-derived carbon for high-performance supercapacitors.
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PubMed
高影响因子
BIOMACROMOLECULES
·
2021
·
IF 6.988
Zhongzheng Ma,Jiake Wang,Yongqi Deng,Yan Wang,Lifeng Yan
A new strategy has been developed to synthesize deep eutectic solvent (DES)-based lignin eutectogels by the chemical crosslinking of homogeneously dispersed lignin with poly(ethylene glycol)diglycidyl ether (PEGDE) in a ternary DES of choline chloride (ChCl)/urea/glycerol. The as-prepared lignin eutectogels have high ionic conductivity, high strength, and extreme temperature stability, which can be used as sensors for flexible electronics. N-doped hierarchical porous carbons (HPCs) are prepared when the eutectogels were solvent-replaced and sintered in the atmosphere of N2 and CO2, which results in the formation of porous carbon with a sufficient specific surface area and a three-dimensional framework composed of a hierarchical porous structure. They were used as electrodes with excellent capacitance performance attributed to the synergy of reasonable pore size distribution and excellent nitrogen doping efficiency. The electrode displayed a significantly enhanced specific capacitance (270 F g–1 at a current density of 1.0 A g–1 in a three-electrode system and 224 F g–1 at 0.5 A g–1 in a two-electrode system) and high-performance stability (7% capacitance loss over 10,000 cycles at 8 A g–1) as a supercapacitor electrode. It indicates the great promise of the lignin eutectogels for both sensing and energy storage applications.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Huihui Xie,Hui Zhang,Xinxin Liu,Shenglong Tian,Yunsi Liu,Shiyu Fu
A lignin-based PU coating was prepared for paper-based green packaging. Two representative diisocyanate were used to prepare the coatings. Due to the rigid aromatic, the physical properties of the TDI system reached the maximum below the lignin content of 40%. The HDI that contains flexible aliphatic chains alleviated the brittleness of coating, and it showed physical advantages when the lignin content was more than 50%. Owing to the high lignin content, the coating presented enhanced thermal stability . After coated with the lignin-based PU coatings, the dry tensile strength of coated paper was improved by 126%. Amazingly, the wet strength was increased from 0.31 to 12.6 MPa with an improvement nearly 40 times. Based on the coordination of lignin, Ag + was introduced into the PU matrix, which imparted the coating with excellent antibacterial ability. The colony forming units of E. coli and S. aureus were both less than 1. However, no inhibition halo was observed, which indicated that the Ag was firmly anchored on the coating and the antibacterial ability is only available when the bacterial contact the coating surface. The lignin-based PU coating with favorable sustainability and properties shows great potential in paper-based green packaging fields.
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PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2021
·
IF 7.033
Zhe Xiong,Yimin Xiong,Qiaoling Li,Hengda Han,Wei Deng,Jun Xu,Long Jiang,Sheng Su,Song Hu,Yi Wang,Jun Xiang
The vapor-/solid-phase interactions are the inevitable phenomenon in biomass pyrolysis process , which significantly affects the formation of heavy components (molecular weight > 200 Da) in bio-oil (HCO). In this study, to deeply understand the mechanism of the formation of HCO during biomass pyrolysis, the effects of the vapor-/solid-phase interactions among cellulose , hemicellulose , and lignin (biomass three components) on the formation of HCO during pyrolysis were studied in a fixed-bed reactor system. The HCO were analyzed by the FT-ICR MS spectrometer and the UV-F spectrometer. The results showed that the vapor-phase interactions mainly promoted the formation of heavy phenolic compounds at a slow heating rate , and the total content of HCO was increased. The vapor-phase interactions decreased the total content and the O content of HCO obviously at a fast heating rate; meanwhile, the highly reactive compounds (e.g., furans, acids, and ketones) generated from the pyrolysis of cellulose and hemicellulose could interact with the phenol monomers . Thus the phenolic compounds were transformed into large aromatic compounds via the vapor-phase interactions. The solid-phase interactions facilitated the transformation of O-containing structures of the HCO into the char via cross-condensation reaction, decreasing the yield of HCO, especially the phenolic compounds and the saccharides .
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