ENERGY & FUELS
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2025
·
IF 5.3
Ajibola T. Ogunbiyi,Wenzhi Li,Leyu Zhu,Amir Hamza,Jingting Jin
Despite lignin’s massive potential for biobased clean fuel production, developing effective catalysts for selectively cleaving its interunit bonds to harness this potential continues to be challenging. In this study, an HZSM-5-supported MoO3 catalyst was developed for a one-pot, hydrothermal kraft lignin depolymerization to maximize liquid fuel yield. A record-high 85.1% yield of petroleum ether-soluble product (a potential gasoline substitute), an unprecedented 45.3% yield of aromatic monomer, and a meager 4.9% char yield (corresponding to a 95.1% lignin conversion) were realized at 300 °C and 24 h in a catalytic transfer hydrogenolysis. The resulting liquid fuel afforded a calorific value of 35.97 MJ/kg, significantly improving over the 25.45 MJ/kg in the original kraft lignin. Catalyst characterization results showed that an optimal acidity characteristic and a suitable Mo-zeolite interaction were pivotal to the efficient cleavage of the C–O and C–C bonds in the kraft lignin. The analyses of the spent catalyst revealed that the formation of inactive Mo4+ species and carbonaceous deposits on the catalyst’s surface was responsible for the initial catalyst deactivation, but recalcination reinstated the catalyst activity. This study extends the frontiers of knowledge in rational catalyst development for lignin valorization applications.
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2024
·
IF 5.3
Wen-luan Xie,Bin Hu,Xiao Yang,Ji Liu,Zhi-mo Fang,Kai Li,Yang-wen Wu,Bing Zhang,Qiang Lu
Phosphoric acid is an effective and widely used catalyst for biomass pyrolysis, with significant catalytic impact on the pyrolytic reactions and product distribution. However, its fundamental catalytic mechanism in lignin pyrolysis remains unclear. In this work, we proposed and investigated three possible H 3 PO 4 -assisted pyrolysis mechanisms, i.e., hydrogen-bond-induced decomposition, phosphoric-acid-assisted hydrogen transfer (H 3 PO 4 -AHT), and phosphorolysis, and carefully discussed them through theoretical calculations, electronic structure analyses, catalytic pyrolysis experiments using the β -O-4 linked lignin model. The results indicated that the H 3 PO 4 -AHT mechanism played a dominant role in lignin catalytic pyrolysis, superior to the other two mechanisms. The phosphoric acid molecule could take advantage of its unsaturated P = O and saturated P −OH groups for hydrogen donation and acceptance in concerted H 3 PO 4 -AHT reactions. Alternatively, it could also participate in concerted intermolecular hydrogen transfer with the active hydroxyl group as a mediator. The C β −O bond cleavage could be significantly enhanced by effectively reducing the tension of the transition state ring, leading to the generation of more phenol and styrene in pyrolysis experiments. Due to the inhibition of hydrogen abstraction, C α −C β breakage of β -O-4 linkage, side chain removal of primary products, etc., the formation of other products in phosphoric acid catalytic pyrolysis of β -O-4 linked lignin was restrained. This H 3 PO 4 -AHT catalytic mechanism was also confirmed to be conductive to tautomerism, elimination, dehydration, α -O-4 linkage fracture, β -1 linkage fracture, and other important decomposition reactions in lignin pyrolysis. The understanding of these mechanisms provides valuable insights into the role of phosphoric acid in lignin pyrolysis and may guide the development of effective biomass catalytic conversion methods.
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PLANT BIOTECHNOLOGY JOURNAL
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2023
·
IF 13.8
Shaozhuo Xu,Manyi Sun,Jia-Long Yao,Xiuxia Liu,Yongsong Xue,Guangyan Yang,Rongxiang Zhu,Weitao Jiang,Runze Wang,Cheng Xue,Zhiquan Mao,Jun Wu
Summary Stone cells are often present in pear fruit, and they can seriously affect the fruit quality when present in large numbers. The plant growth regulator NAA, a synthetic auxin, is known to play an active role in fruit development regulation. However, the genetic mechanisms of NAA regulation of stone cell formation are still unclear. Here, we demonstrated that exogenous application of 200 μ M NAA reduced stone cell content and also significantly decreased the expression level of PbrNSC encoding a transcriptional regulator. PbrNSC was shown to bind to an auxin response factor, PbrARF13. Overexpression of PbrARF13 decreased stone cell content in pear fruit and secondary cell wall (SCW) thickness in transgenic Arabidopsis plants. In contrast, knocking down PbrARF13 expression using virus-induced gene silencing had the opposite effect. PbrARF13 was subsequently shown to inhibit PbrNSC expression by directly binding to its promoter, and further to reduce stone cell content. Furthermore, PbrNSC was identified as a positive regulator of PbrMYB132 through analyses of co-expression network of stone cell formation-related genes. PbrMYB132 activated the expression of gene encoding cellulose synthase ( PbrCESA4b/7a/8a) and lignin laccase ( PbrLAC5 ) binding to their promotors. As expected, overexpression or knockdown of PbrMYB132 increased or decreased stone cell content in pear fruit and SCW thickness in Arabidopsis transgenic plants. In conclusion, our study shows that the ‘PbrARF13-PbrNSC-PbrMYB132’ regulatory cascade mediates the biosynthesis of lignin and cellulose in stone cells of pear fruit in response to auxin signals and also provides new insights into plant SCW formation.
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PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Shengwei Cheng,Jinhui Lin,Jundong Si,Jie Yin,Longgui Zhang,Xiangchen Fang,Yan Zhang
Branched poly(butylene succinate- co -terephthalate) (PBST)-based composites, a kind of bioplastic incorporated with lignin and other auxiliary agents with excellent mechanical properties, were obtained through melting processing in this work. Wherein, the epoxy group in multifunctional styrene-acrylic-epoxy-based random oligomer chain extender Joncryl ADR-4468 (ADR) could react in situ with hydroxyl in lignin and branched PBST. Additionally, Zn 2+ from zinc stearate (ZnSt) could form metal coordination bonds with the oxygen-containing functional groups of lignin and branched PBST. The in situ reaction and metal coordination bonds could improve the compatibility of the two. The tensile strength and the elongation at break could reach 18.6 MPa and 1224.7%, respectively, because of the increased compatibility. Moreover, the composites also exhibited hydrophobicity, excellent UV resistance, and visible light barrier properties. It is expected to have broad application prospects in the fields of agricultural mulch film and packaging.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
·
IF 8.5
Xinyue Wang,Tengteng Zhang,Jinfang Chu,Wei Ding,Zekun Wang,Xuehai Gong,Yushun Jin,Ruofan Liu,Yibo Wu
As the most abundant natural aromatic polymer, lignin demonstrates unparalleled potential in advancing sustainable waterborne polyurethane (WPU) systems. This work redefined the role of enzymatic lignin (EL) by strategically integrating it as a chain extender (C-LWPU) and a reinforcing filler (F-LWPU), transcending its conventional use as a filler. When employed as a chain extender, EL enabled a remarkable incorporation of 20 wt%, yielding LWPU films with a tensile strength of 31.73 MPa, a 772 % enhancement over pristine WPU, along with exceptional bioactivity (free radical scavenging ratios of 99.4 % for ABTS + and 91.3 % for DPPH), superior UV shielding, and thermal stability. In contrast, the F-LWPU films achieved a marginally higher tensile strength (34.37 MPa) but required only 1 wt% EL loading, while with reduced bioactivity (free radical scavenging ratios of 92.1 % for ABTS + and 20.9 % for DPPH). Crucially, the C-LWPU system outperformed in balancing high EL utilization, cost-effectiveness, and multifunctionality, underscoring EL's capacity to act as a multifunctional structural unit rather than a mere filler. By resolving the longstanding trade-off between high biomass content and performance, this work establishes EL as a pivotal enabler of next-generation WPU materials, offering a scalable pathway toward fully bio-based polymers with tailored properties for industrial applications.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Haozhi Zhang,Qian Sun,Yi-Bing Liu,Cheng-Ye Ma,Jia-Long Wen,Zhenglong Li,Tong-Qi Yuan
Efficient fractionation of reed biomass and tailored downstream high value-added applications are crucial for biorefining sustainability. To address the issues of hemicelluloses non-recovery and lignin structure destruction during DES pretreatment, a green and efficient alkaline deep eutectic solvent (ADES) pretreatment strategy was developed. The strategy aims to achieve efficient fractionation of reed biomass, while providing uncondensed lignin, hemicelluloses with high structural retention, and easily digestible cellulose residues for bioenergy and chemicals. Results demonstrated that the proposed ADES pretreatment strategy exhibited excellent capability in deconstructing biomass component, achieving a delignification efficiency of 82.95 wt%-96.13 wt% (ADES-NAP/CAP/CEM systems at 120–160 °C for 10 min). Meanwhile, lignin fractions had excellent antioxidant activity and well-preserved structure (high content of β- O -4 aryl ether bonds), which facilitated to the development of downstream applications and monomer production (29.34 wt%-41.16 wt% via reductive catalytic degradation at 180–260 °C). On the other hand, the pretreatment efficiently removed hemicelluloses (83.49 wt%-97.61 wt%), while enabling the recovery of high-purity hemicelluloses with structural integrity well-preserved. The ADES cellulose residues achieved 60.39 wt%-97.68 wt% fermentable glucose yield at low enzyme loading (10 FPU/g) during enzymatic saccharification, with a total biorefinery yield exceeding 81 %. In summary, the proposed ADES pretreatment strategy not only solved the problem of hemicelluloses degradation during DES pretreatment but also realized efficient separation, conversion and utilization of all components within reed biomass.
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高影响因子
Processes
·
2025
·Vol. 14
·期 1
·55
·
IF 2.8
Bao Fan,Jiale Xiong,Cuiluan Ma,Yu-Cai He
Gastrodin is a bioactive component of traditional Chinese medicine, exhibiting anti-cancer, anti-inflammatory, antioxidant and neuroprotective properties. It has broad application prospects in health foods, pharmaceuticals and cosmetics. In recent years, the conversion of biomass-derived aldehydes into high-value-added chemicals has garnered widespread attention. In this study, gastrodin was biosynthesized via a dual-enzyme coupling system consisting of UGTBL1-Δ60 and KpADH. Specifically, lignin-derivedp-hydroxybenzaldehyde was used as the substrate. First, the glycosylation ofp-hydroxybenzaldehyde by UGTBL1-Δ60 yieldedp-hydroxybenzaldehydeβ-glucoside, generating the glycosylation reaction solution. Subsequently, bioreduction of the glycosylation product by KpADH produced gastrodin. Under the optimal reaction conditions (0.05 g/mL KpADH whole cells, 50 mM glucose, pH 7.5 and 30 °C) a gastrodin yield of 82.8% was achieved within 12 h. Moreover, both UGTBL1-Δ60 and KpADH retained high catalytic activity after multiple reaction cycles. This study establishes a green and efficient biocatalytic approach for gastrodin synthesis, and also provides new insights into the high-value utilization of lignin.
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ACS Sustainable Chemistry & Engineering
·
2022
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IF 9.224
Zhan-Chao Li,Wei Li,Dong-Xia Wang,Rui Wang,An-Na Tang,De-Ming Kong
To reduce poverty and hunger in economically backward countries and regions, increasing demand for addressing severe worldwide food deterioration and wastage has triggered intensive research efforts toward modified atmosphere packaging (MAP) technology. Herein, we demonstrate that natural lignin can be used as a cheap and green monomer for preparation of hydrogen-bonded covalent organic polymers (HCOPs) with good crystallinity, permanent porosity, and high thermostability. The optimal lignin-based HCOPs (named LT-HCOPs) are synthesized by using tetrafluoroterephthalonitrile as the cross-linker, ethanol/water (7/3, v/v) as the reaction solvent, 120 °C as the reaction temperature, and ammonium persulphate and anhydrous potassium carbonate as catalysts. As-prepared LT-HCOPs can be used as promising “switches” for regulating gas permeability in the passive MAP membranes. The LT-HCOP-based passive MAP membrane, which is prepared by a simple mixing and solvent evaporation process, shows good biocompatibility, antimicrobial and antioxidant activities, improved ultraviolet light barrier property, high CO2/O2 selectivity, and suitable H2O permeation and thus is demonstrated to work well in prolonging the shelf life of perishable foods such as strawberries, waxberries, cherries, cherry tomatoes, and mangoes. This work provides a feasible way to use cheap and green natural materials to construct advanced functional materials for practical applications.
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ENERGY & FUELS
·
2019
·
IF 3.021
Yunfei Bai,Kai Cui,Yushuai Sang,Kai Wu,Fei Yan,Fuhang Mai,Zewei Ma,Zhe Wen,Hong Chen,Mengmeng Chen,Yongdan Li
A one-pot process for the depolymerization of lignin-rich corncob residue (LRCR) is investigated in supercritical ethanol over an alumina-supported NiMo (NiMo/Al) alloy catalyst. The LRCR, as a major byproduct in the corncob enzymatic hydrolysis process, was completely liquefied and effectively transformed into aromatic compounds without the formation of tar or char under optimal reaction conditions. The reaction temperature, time, solvent, and initial hydrogen pressure have significant effects on the depolymerization of LRCR. The highest overall aromatic yield of 255.4 mg/g of LRCR with 57.9 wt % alkylphenols (e.g., 4-ethylphenol, 2,5-diethylphenol, and 2,6-diisopropylphenol) was achieved with an initial 27.6 bar (gauge) of hydrogen in supercritical ethanol at 320 °C for 7.5 h. The depolymerization of LRCR is also examined over Ni/γ-Al2O3, Mo/γ-Al2O3, and the physical mixture of these two catalysts. The NiMo/Al alloy catalyst exhibits much higher activity than that of other catalysts, and a synergistic effect between Ni and Mo active species is proposed. Furthermore, X-ray powder diffraction results show that the Mo1.24Ni0.76 alloy is expected to be an important active species for the depolymerization reaction.
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Journal of Energy Chemistry
·
2020
·
IF 7.216
Pengfei Lu,Fangyan Liu,Feng Zhou,Jieqiong Qin,Haodong Shi,Zhong-Shuai Wu
Lithium–selenium (Li–Se) batteries have attracted considerable attentions for next-generation energy storage systems owing to high volumetric capacity of 3265 mAh cm −3 and excellent electronic conductivity (~10 −5 S cm −1 ) of selenium. However, the shuttling effect and capacity fading prevent their wide applications. Herein we report a low-cost strategy for scalable fabrication of lignin derived hierarchical porous carbon (LHPC) as a new high-loading Se host for high-capacity and long-term cycling Li–Se batteries in carbonate electrolyte. The resulting LHPC exhibits three-dimensional (3D) hierarchically porous structure, high specific surface area of 1696 m 2 g −1 , and hetero-atom doping (O, S), which can effectively confine the Se particles into the micropores, and meanwhile, offer effective chemical binding sites for selenides from hetero-atoms (O, S). As a result, our Li–Se batteries based on Se@LHPC demonstrate high capacity of 450 mAh g −1 at 0.5 C after 500 cycles, with a low capacity fading rate of only 0.027%. The theoretical simulation confirmed the strong affinity of selenides on the O and S sites of LHPC effectively mitigating the Se losing. Therefore, our strategy of using lignin as the low-cost precursor of hierarchically porous carbon for high-loading Se host offers new opportunities for high-capacity and long-life Li–Se batteries.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2019
·
IF 4.784
Xueming Bao,Xuerong Fan,Yuanyuan Yu,Qiang Wang,Ping Wang,Jiugang Yuan
In this study, a green approach combining enzyme-initiated reversible addition-fragmentation chain transfer (RAFT) polymerization and free-radical coupling was developed for the modification of jute fiber , which is a typical lignin-based cellulose. Jute fiber surface was covered by rich amount of lignin, which offered great opportunities for further functional modification. The controlled polymerization of vinyl monomers , acrylamide (AM) or butyl acrylate (BA), was carried out by horseradish peroxidase (HRP)-initiated RAFT to form well-defined polymers with well-controlled molecular weights and structures. Enzymatic grafting by HRP occurred between the free radicals of well-defined polymers and free radicals of lignin on jute. Gel permeation chromatography (GPC) analysis indicated the alkyl chain length of polymers prepared via HRP-initiated RAFT polymerization was well-controlled. Other results of flourier transformed infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) revealed that well-controlled alkyl chains prepared via enzymatic catalysis were grafted on the exposed lignin of jute. The study explores a new and eco-friendly modification method for lignin-based materials with the controlled graft chain structure via two different catalysis with HRP.
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ACS Omega
·
2022
·
IF 4.132
Haonan Cong,Zihao Ma,Meixi Hu,Junjie Han,Xing Wang,Ying Han,Yao Li,Guangwei Sun
Herein, we developed an efficient and convenient method to address the problem of thickener decomposition in the low- permeability oilfield production process. It is crucial to design breakers that reduce viscosity by delaying thickener decomposition in appropriate environments. By using lignin in biomass as a substrate for β-mannanase immobilization (MIL), we fabricated a gel breaker, surface gelatin-coated β-mannanase-immobilized lignin (Ge@MIL). Through experiments and performance tests, we confirmed that the prepared Ge@MIL can release enzymes at a specific temperature, meanwhile having temperature-sensitive phase change properties and biodegradability. The results also show the tight tuning over the surface coating of Ge@MIL by a water-in-oil emulsion. Therefore, the prepared Ge@MIL has a promising application in the field of oil extraction as a green and efficient temperature-sensitive sustained-release capsule.
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