Deep Eutectic Solvent Pretreatment Research Articles

Synergism of jet milling and deep eutectic solvent pretreatment on grapevine lignin fractionation and enhancing enzymatic hydrolysis

Herein, we investigated the synergistic effects of jet milling (JM) and deep eutectic solvent (DES) pretreatment on the fractionation of grapevine lignin and the consequent enhancement of enzymatic hydrolysis. Grapevine, a substantial byproduct of the wine industry, was subjected to JM pretreatment to produce finely powdered particles (median diameter D50 = 98.90), which were then further treated with acidic ChCl-LA and alkaline K2CO3-EG DESs. The results revealed that the combined JM + ChCl-LA pretreatment significantly increased the cellulose preservation under optimal conditions (110 °C, 4 h, and 20 % water content), achieving removal rates of 74.18 % xylan and 66.05 % lignin, respectively. The pretreatment temperature and inhibitor production were reduced, resulting in a remarkable threefold increase in glucose yield compared to untreated samples. Moreover, the structural analysis of the pretreated lignin indicated an enrichment of phenolic units, leading to enhanced antioxidant and antibacterial activities, particularly in the JM pretreated samples. These findings underscore the promising potential of the synergistic JM and DES pretreatment in facilitating the efficient utilization of grapevine lignocellulosic biomass for sustainable biorefinery technologies.

Facilitating the fabrication of diverse bio-based nanomaterials from bamboo using one-pot hydrated deep eutectic solvent pretreatment

The conversion of biomass feedstocks into bio-based nanomaterials was made easier with hydrated DES (HDES) pretreatment, which can boost the value-added applications of lignocellulosic biomass. In this study, two types of HDESs were initially prepared by 3-Chloro-2-hydroxypropyltrimethyl ammonium chloride (CHPTAC) with formic acid (FA) and acetic acid (AA), respectively. We achieved rapid conversion of bamboo feedstock into bio-based nanomaterials (including lignin nanoparticles, LNPs; lignin-containing cellulose nanofibers, LCNFs) through one-pot microwave-assisted HDES pretreatment coupled with robust nanofabrication strategies. The findings demonstrated that an impressive delignification ratio of 92.10 % and a cellulose retention ratio of 92.95 % were achieved under the optimal DES pretreatment conditions (120 °C, 20 min). The fractionated lignin fractions were effortlessly self-assembled into dispersed, uniformly shaped circular LNPs (<100 nm) using a novel proposed strategy, which was successfully applied to stabilizing oil-in-water (O/W) Pickering emulsions. To produce LCNFs, we conducted functionalization of cellulose-rich residue in aqueous citric acid followed by simple ultrasonic treatment. Compared to the control LCNF, the LCNF-based self-assembly films exhibited significantly improved mechanical properties and hydrophobicity (water contact angle 106.26°). In short, the proposed HDES pretreatment combined with robust nanofabrication strategies will broaden the fractionation and fabrication of bio-based nanomaterials, enhancing their potential in promising fields.

Deep eutectic solvent pretreatment of sugarcane bagasse for efficient lignin recovery and enhanced enzymatic hydrolysis

This study explores the sugarcane bagasse (SCB) pretreatment with two deep eutectic solvents (DESs) prepared from choline chloride (ChCl) as a hydrogen bond acceptor (HBA) to two hydrogen bond donors (HBD): oxalic acid (OA) and trifluoroacetic acid (TFA) for lignin recovery and enhancing enzymatic saccharification. The pretreatment conditions, reaction time, temperature, and DES concentration were optimized using response surface methodology. The two DESs showed a lignin yield of 74.67 ± 2.75 and 83.50 ± 2.65 mg per gm of SCB, respectively. Enzymatic hydrolysis of the cellulose-enriched material (CEM) obtained after pretreatment showed an enhanced RS yield of around 4-fold compared to the untreated SCB. The CEM was characterized using FTIR, Powder X-ray diffraction, and Scanning Electron Microscopy. The recovered lignin characteristics were studied using FTIR, 1H NMR, and 2D-HSQC NMR analysis. The FTIR spectra of lignin show the presence of aromatic skeletal vibrations, -OH, -CH, C-O stretching vibration, and aromatic C-H deformation. Furthermore, the pretreatment solvent recyclability studies were conducted to evaluate the effectiveness of DES for a sustainable biorefinery process.

Current progress on lignocellulosic bioethanol including a technological and economical perspective

AbstractGrowing interest in lignocellulosic bioethanol stems from the European Union's renewable energy directive, targeting a global bioethanol output of 130 billion L to achieve a minimum threshold of 42.5%. Despite industrialization challenges, recent advancements, especially in crucial stages like pretreatment, hydrolysis, and fermentation, are transforming the landscape. This review delves into the progress of bioethanol production, addressing technological, environmental, and economic hurdles. Innovations such as deep eutectic solvent pretreatment and mechanocatalysis, offering advantages like 30% and 100% solid loading, respectively, surpass traditional techniques and enzymatic hydrolysis in yielding better results. Improved pretreatment methods, enzyme exploration, saccharification techniques, genetic engineering, and integrated biorefineries contribute to overall economic viability. Ongoing research involves techno-economic analysis for cost-effective strategies, aiming to enhance the competitiveness of lignocellulosic bioethanol production. Scrutinizing the feasibility of these innovative approaches not only highlights their potential to overcome existing shortcomings but also envisions a more attractive future for industrial bioethanol production. Embracing these advancements could pave the way for a vibrant and sustainable bioethanol industry.

Synthesis and characterization of composite films derived from lemongrass leaves: A valorization approach

Over the past few decades, research into more ecologically friendly packaging materials has significantly increased to reduce non-renewable plastic usage. In this context, biobased films were synthesized from extracted lemongrass leaves. An integrated pretreatment of conventional alkali followed by deep eutectic solvents (DES) was utilized to fractionate the lemongrass leaves into three usable forms, i.e., hemicellulose (HC), lignin (L), and cellulose, which were further utilized in the synthesis of composite films. A total of 4 films have been synthesized, labelled as: Film 1 (CMC HC), Film 2 (L HC), Film 3 (CMC L), and Film 4 (CMC HC L). Film 4 has shown a good water absorption capacity of nearly 65 % and also a higher contact angle of 99.90°, while film 2 has the highest thermal stability among all the films. Film 3 has better UV properties due to the presence of carboxymethyl cellulose (CMC) and lignin. Statement of noveltyIn the present work, composite films have been synthesized from lemongrass leaves for the first time. This is the first report that synthesizes the films from extracted components (CMC, lignin, and hemicellulose) of lemongrass leaves. In this study, all the components were extracted via sequential conventional alkali and DES pretreatment. After extraction, these components were utilized for the composite film synthesis, which is used for various applications of their desirable properties.

A novel seawater hydrothermal-deep eutectic solvent pretreatment enhances the production of fermentable sugars and tailored lignin nanospheres from Pinus massoniana

Lignocellulose biorefinery depended on effective pretreatment strategies is of great significance for solving the current global crisis of ecosystem and energy security. This study proposes a novel approach combining seawater hydrothermal pretreatment (SHP) and microwave-assisted deep eutectic solvent (MD) pretreatment to achieve an effective fractionation of Pinus massoniana into high value-added products. The results indicated that complex ions (Mg2+, Ca2+, and Cl−) in natural seawater served as Lewis acids and dramatically promoted the depolymerization of mannose and xylan into oligosaccharides with 40.17 % and 75.43 % yields, respectively. Subsequent MD treatment realized a rapid and effective lignin fractionation (~90 %) while retaining cellulose. As a result, the integrated pretreatment yielded ~85 % of enzymatic glucose, indicating an eightfold increase compared with untreated pine. Because of the increased hydrophobicity induced by the formation of acyl groups during MD treatment, uniform lignin nanospheres were successfully recovered from the DES. It exhibited low dispersibility (PDI = 2.23), small molecular weight (1889 g/mol), and excellent oxidation resistance (RSI = 5.94), demonstrating promising applications in functional materials. The mechanism of lignin depolymerization was comprehensively elucidated via FTIR, 2D-HSQC NMR, and GPC analyses. Overall, this study provides a novel and environmentally friendly strategy for lignocellulose biorefinery and lignin valorization.

Synergistic microwave and acidic deep eutectic solvent-based pretreatment of Theobroma cacao pod husk biomass for xylooligosaccharides production

The bioconversion of lignocellulosic biomass into novel bioproducts is crucial for sustainable biorefineries, providing an integrated solution for circular economy objectives. The current study investigated a novel microwave-assisted acidic deep eutectic solvent (DES) pretreatment of waste cocoa pod husk (CPH) biomass to extract xylooligosaccharides (XOS). The sequential DES (choline chloride/citric acid, molar ratio 1:1) and microwave (450W) pretreatment of CPH biomass was effective in 67.3% xylan removal with a 52% XOS yield from total xylan. Among different XOS of varying degrees of polymerization, a higher xylobiose content corresponding to 69.3% of the total XOS (68.22 mg/g CPH) from liquid fraction was observed. Enzymatic hydrolysis of residual xylan from pretreated CPH biomass with low commercial xylanase (10 IU/g) concentration yielded 24.2% XOS. The MW-ChCl/citric acid synergistic pretreatment approach holds great promise for developing a cost-effective and environmentally friendly method contributing to the sustainable production of XOS from agricultural waste streams.

Efficient extraction of lignin from moso bamboo by microwave-assisted ternary deep eutectic solvent pretreatment for enhanced enzymatic hydrolysis

Applications of deep eutectic solvent (DES) systems to separate lignocellulosic components are of interest to develop environmentally friendly processes and achieve efficient utilization of biomass. To enhance the performance of a binary neutral DES (glycerol:guanidine hydrochloride), various Lewis acids (e.g., AlCl3·6H2O, FeCl3·6H2O, etc.) were introduced to synthesize a series of ternary DES systems; these were coupled with microwave heating and applied to moso bamboo. Among the ternary DES systems evaluated, the FeCl3-based DES effectively removed lignin (81.17%) and xylan (85.42%), significantly improving enzymatic digestibility of the residual glucan and xylan (90.15% and 99.51%, respectively). Furthermore, 50.74% of the lignin, with high purity and a well-preserved structure, was recovered. A recyclability experiment showed that the pretreatment performance of the FeCl3-based DES was still basically maintained after five cycles. Overall, the microwave-assisted ternary DES pretreatment approach proposed in this study appears to be a promising option for sustainable biorefinery operations.

Optimizing invasive plant biomass valorization: Deep eutectic solvents pre-treatment coupled with ZSM-5 catalyzed fast pyrolysis for superior bio-oil quality

The primary objective of this study is to explore the application of a deep eutectic solvent, synthesized from lactic acid and choline chloride, in combination with a pre-treatment involving ZSM-5 catalytic fast pyrolysis, aimed at upgrading the quality of bio-oil. Characterization results demonstrate a reduction in lignin content post-treatment, alongside a significant decrease in carboxyls and carbonyls, leading to an increase in the C/O ratio and noticeable enhancement in crystallinity. During catalytic fast pyrolysis experiments, the pre-treatment facilitates the production of oil fractions, achieving yields of 54.53% for total hydrocarbons and 39.99% for aromatics hydrocarbons under optimized conditions. These findings validate the positive influence of the deep eutectic solvent pre-treatment combined with ZSM-5 catalytic fast pyrolysis on the efficient production of bio-oil and high-value chemical derivatives..

The full utilization of bagasse via deep eutectic solvent pretreatment for low-condensed lignin and cellulose smart indicator film

Full utilization of biomass after fractionation of its components is an effective way to maximize the value of biomass. Herein, in this study, a new acetal-mediated deep eutectic solvent (DES) was explored and its excellent performance in separating lignin from biomass as well as retarding lignin condensation has been observed. Subsequently, the separated lignin and cellulose-rich residue were used to prepare sunscreen and transparent food indicator films, respectively. The results showed that the acetal-mediated DES pretreatment can reduce the recalcitrance of bagasse, stabilize lignin (β-O-4 content of 68.87% in the lignin), and retain most of the cellulose (ie. 83.5%). Besides, the pretreatment enhanced the subsequent hydrogenolysis of lignin, and the higher β-O-4 content of the lignin contributed to the high yield of aromatic monomers (40.94%). In addition, regenerated lignin was attractive for sunscreen applications due to its lighter color and excellent UV-blocking properties. Furthermore, cellulose smart indicator film was highly sensitive, biodegradable, has excellent physical properties, and allows visual real-time monitoring of seafood spoilage using smartphones. Meanwhile, the yield of the removed hemicellulose converted to xylose in the pretreatment process reached 99.41%. In general, this work proposed a sustainable bio-refinery approach for the full upgrading of biomass.

Process design for acidic and alcohol based deep eutectic solvent pretreatment and high pressure homogenization of palm bunches for nanocellulose production

This research aimed to study on nanocellulose production from palm bunch using process design and cost analysis. Choline chloride based deep eutectic solvent pretreatment was selected for high-purity cellulose separation at mild condition, followed by nano-fibrillation using mechanical treatment. Three types of choline chloride-based deep eutectic solvents employing different hydrogen-bond donors (HBDs) namely lactic acid, 1,3-butanediol and oxalic acid were studied. The optimal cellulose extraction condition was choline chloride/lactic acid (ChLa80C) pretreatment of palm empty bunch at 80 °C followed by bleaching yielding 94.96%w/w cellulose content in product. Size reduction using ultrasonication and high-pressure homogenization produced nanocellulose at 67.12%w/w based on cellulose in raw material. Different morphologies of nanocellulose were tunable in the forms of nanocrystals, nano-rods and nanofibers by using dissimilar deep eutectic solvents. This work offered a sustainable and environmentally friendly process as well as provided analysis of DES pretreatment and overview operating cost for nanocellulose production. Application of nanocellulose for the fabrication of highly functional and biodegradable material for nanomedicine, electronic, optical, and micromechanical devices is achievable in the near future.

Deep eutectic solvents pretreatment enhances methane production from anaerobic digestion of waste activated sludge: Effectiveness evaluation and mechanism elucidation

Anaerobic digestion (AD) is a prevalent waste activated sludge (WAS) treatment, and optimizing methane production is a core focus of AD. Two DESs were developed in this study and significantly increased methane production, including choline chloride-urea (ChCl-Urea) 390% and chloride-ethylene glycol (ChCl-EG) 540%. Results showed that ChCl-Urea mainly disrupted extracellular polymeric substances (EPS) structures, aiding in initial sludge solubilization during pretreatment. ChCl-EG, instead, induced sludge self-driven organic solubilization and enhanced hydrolysis and acidification processes during AD process. Based on the extent to which the two DESs promoted AD for methane production, the AD process can be divided into stage Ⅰ and stage Ⅱ. In stage Ⅰ, ChCl-EG promoted methanogenesis more significantly, microbiological analysis showed both DESs enriched aceticlastic methanogens-Methanosarcina. Notably, ChCl-Urea particularly influenced polysaccharide-related metabolism, whereas ChCl-EG targeted protein-related metabolism. In stage Ⅱ, ChCl-Urea was more dominant than ChCl-EG, ChCl-Urea bolstered metabolism and ChCl-EG promoted genetic information processing in this stage. In essence, this study investigated the microbial mechanism of DES-enhanced sludge methanogenesis and provided a reference for future research.

A tailored deep eutectic solvent for high-yield conversion of poplar residues to bio-based building blocks at mild conditions

The generation of condensed compounds in a deep eutectic solvent (DES) pretreatment has become a paramount factor that inhibits the further conversion of pretreated cellulose-rich substrate. This study proposed a novel three-constituent DES system for the value-added utilization of poplar residues by efficiently suppressing hemicellulose derived condensation reactions. The results showed that adding ethanol into the DES system could effectively deconstruct the recalcitrant structure of poplar residues, simultaneously hindering the condensed composition formation. Under optimum ethanol addition (30%), the maximum xylan and lignin removal of 87.94% and 90.99% could be achieved, with more than 90.47% of glucan being preserved. With this, the glucan enzymatic hydrolysis efficiency was remarkably improved to 100% under the pretreatment conditions of 100 °C for 60 min, which was 84.69 times higher than the regular DES-pretreated poplar residues (1.17%). The working mechanism of relieving condensation reactions was characterized by Py-GC–MS, NMR, SEM, FTIR, and others. The results demonstrated that the addition of ethanol could regulate the degradation/conversion pathway of hemicellulose and lignin precipitation, thus inhibit the formation of condensed compounds during the pretreatment.

Efficient fractionation of corn stover using deep eutectic solvent from lignin-derived 3-phenylpropionic acid: Towards a closed-loop biorefinery

The search for renewable deep eutectic solvents (DESs) for efficient biomass pretreatment based on a closed-loop biorefinery is of great interest and importance. Herein, we reported three novel lignin-based DESs prepared by choline chloride (ChCl) and 3-(4-hydroxyphenyl)propionic acid (HPA), 3-(4-hydroxy-3-methoxyphenyl)propanoic acid (HMPA) and their combination for corn stover pretreatment. The effects of three lignin-based DESs pretreatments on the chemical compositions of raw material, structural features of lignin, and enzymatic digestibility of cellulose were comprehensively analyzed, among which ChCl/HPA DES exhibited superior pretreatment efficiency, affording 58% of delignification, 62% of hemicellulose removal, and 85% of glucose yield. A high abundance of p-coumaric acid in the regenerated and remaining lignin samples makes them a sustainable feedstock to produce hydrogen bond donors of ChCl/HPA DES, as demonstrated by the results from 2D HSQC NMR analysis and catalytic depolymerization of lignins. These results could be conducive to creating an integrated biorefinery strategy for biomass valorization. Mass balance analysis indicated 81% of cellulose, 90% of hemicellulose, and 91% of lignin components in corn stover could be collected after DES pretreatment. This contribution offers a novel and efficient pretreatment method for corn stover fractionation based on a closed-loop biorefinery.

Promoting the disassemble and enzymatic saccharification of bamboo shoot shells via efficient hydrated alkaline deep eutectic solvent pretreatment

Pretreatment is a key process restricting the development of biorefinery. This work developed a pretreatment process based on an ethanolamine/acetamide alkaline deep eutectic solvent (ADES). Under microwave assistance, pure ADES pretreatment at 100 °C for 10 min achieved 95.9 % delignification and 95.2 % hemicellulose removal of bamboo shoot shells (BSS). Further, when 75 % water was added to pure DES to prepare hydrated DES (75 %-HADES), impressive delignification (93.2 %), hemicellulose removal (92.2 %) and cellulose recovery (94.8 %) were still achieved. The cellulose digestibility of the 75 %-HADES pretreated solid residue was significantly increased from 12.2 % (the control) to 91.2 %. Meanwhile, the structural features of hemicellulose and lignin macromolecules fractionated by 75 %-HADES pretreatment were well preserved, offering opportunities for downstream utilization. Overall, this work proposes an effective pretreatment strategy with the potential to enable the utilization of all major components of bamboo shoot shells.

Improving saccharification efficiency of corn stover through ferric chloride-deep eutectic solvent pretreatment

An effective deep eutectic solvent (DES) and Iron(III) chloride (FeCl3) combination pretreatment system was developed to improve the removal efficiency of lignin and hemicellulose from corn stover (CS) and enhance its saccharification. N-(2-hydroxyethyl)ethylenediamine (NE) was selected as the hydrogen-bond-donor for preparing ChCl-based DES (ChCl:NE), and a mixture of ChCl:NE (60 wt%) and FeCl3 (0.5 wt%) was utilized for combination pretreatment of CS at 110 ℃ for 50 min. FeCl3/ChCl:NE effectively removed lignin (87.0 %) and xylan (55.9 %) and the enzymatic hydrolysis activity of FeCl3/ChCl:NE-treated CS was 5.5 times that of CS. The reducing sugar yield of pretreated CS was 98.6 %. FeCl3/ChCl:NE significantly disrupted the crystal structure of cellulose in CS and improved the removal of lignin and hemicellulose, enhancing the conversion of cellulose and hemicellulose into monomeric sugars. Overall, this combination of FeCl3 and DES pretreatment methods has high application potential for the biological refining of lignocellulose.

Combination of microwave with acid deep eutectic solvent pretreatment for reed (Phragmites australis) fractionation

The cost-effective and low-carbon fractionation of lignocellulosic biomass will enhance the economic viability of bio-refining. To achieve efficient reed fractionation under favorable conditions, microwave-assisted choline chloride and p-toluene sulfonic acid (M-ChCl/p-TsOH) pretreatment was employed. The fractionation of reed components demonstrated higher effectiveness with M-ChCl/p-TsOH pretreatment compared to conventional DES pretreatment. Under M-ChCl/p-TsOH conditions, a high hemicellulose removal rate (∼90%) and delignification rate (∼65%) were achieved while achieving a saccharification rate of 88% during cellulase hydrolysis. Microwave assistance not only significantly reduced reaction time to less than 60 s but also enhanced the pretreatment efficacy. Furthermore, the obtained lignin products consisted of low-polymerization lignin (MW < 800 g/mol) and acid-soluble lignin, providing a solid foundation for subsequent high-value utilization of lignin. This study provides a promising strategy for the low carbon fractionation of reed using DES, aiming to simultaneously achieve efficient cellulose hydrolysis and obtain tractable lignin.

Investigation into the characteristics of bagasse processed with 3C-DES and the production of chemimechanical pulp for pulp molded

Pulp molded generated from renewable bagasse as biodegradable packaging materials has been widely viewed as an eco-friendly and cheap way to substitute the current huge consumption of nondegradable plastics, and deep eutectic solvents (DES) pretreatment are a promising approach to obtain high-yield pulp efficiently and sustainably. However, mainstream binary-component DES still suffers issues of high viscosity and corrosiveness. This study put forward a ternary-component DES (3C-DES) with the addition of ethylene glycol (EG) into choline chloride (ChCl) and P-toluenesulfonic acid (PTSA) and examined pretreatment performance and optimal DES ratio for thread rolling bagasse via compositional analysis and physicochemical characterization. Moreover, density functional theory calculations were used to reveal structures and weak interactions of different ratios of 3C-DES, and a novel 3C-DES pretreatment chemical-mechanical pulp and pulp molded were finally prepared. The results indicate that the 3C-DES with ChCl:PTSA:EG molar ratio of 1:1:3 is most effective, evidenced by more than 97.94% lignin removals. The 3C-DES pretreated mechanical pulp exhibits superior fiber properties, whereas the hot-pressed pulp molded shows excellent physical properties and thermal stability. Thus, the proposed 3C-DES has great potential to obtain high-yield high-performance pulp molded with low cost and environmental sustainability.

Oxidized cellulose as bio‐adhesive for hydrophobic lignocellulosic bioplastic

AbstractThis study presents a novel hydrophobic lignocellulosic bioplastic from corn stover reinforced by oxidized cellulose and in situ regenerated lignin. Cellulose‐lignin mixture as a matrix was obtained by acid‐recyclable deep eutectic solvent (DES) pretreatment of corn stover in mild conditions. Triethoxy(octyl)silane (C14H32O3Si) was employed to improve the water stability of the bioplastic by vapor deposition. The results show that the hydrophobic bioplastic has a high tensile strength, measuring 62.36 MPa. The water contact angle of the bioplastic was increased from 8.50° to 121.9° after hydrophobic modification. We prepared oxidized cellulose‐reinforced cellulose paper by different particle size distributions of oxidized cellulose to investigate the reinforcement of oxidized cellulose. The tensile strength of oxidized cellulose cellulose paper increased from 14.41 to 21.18 MPa with the addition of oxidized cellulose. The zeta potential of oxidized cellulose is −47.99 mV, which shows a more negative charge due to carbonyl groups. The repulsive force of oxidized cellulose contributes to the formation of a brick‐and‐mortar microstructure with cellulose‐lignin mixture. It demonstrates that oxidized cellulose can act as bio‐adhesives and has a good toughening effect on the mechanical properties of bioplastic.Highlights Lignocellulosic bioplastic was prepared by DES pretreatment of corn stover. Oxidized cellulose was used to reinforce the lignocellulosic bioplastic. The tensile strength of the bioplastic was 62.36 MPa after the reinforcement process. Trieth‐oxy(octyl)silane was employed to improve water stability. The water contact angle of the bioplastic was increased from 8.50° to 121.9°.

Cascade fractionation of bamboo shoot shells into high-yield xylose, easily digestible cellulose and high-quality lignin nanoparticles by tailored catalytic hydrothermal–hydrated alkaline deep eutectic solvents pretreatment

The high complexity and compactness of inherent structure in lignocellulosic materials (LCM) leads to the difficulty of fractionation and conversion of its major component, which is the key obstacle limiting the value-added utilization of LCM. In this work, a cascade fractionation strategy, coupling catalytic hydrothermal pretreatment (CHTP, choline chloride: ethylene glycol: AlCl3, ChCl/ EG/ AlCl3) with hydrated alkaline deep eutectic solvent (HADES, triethylbenzyl ammonium chloride/ethanolamine, TEBAC/EM) treatment, was proposed to fractionate dendrocalamus latiftorus munro shoot shells (DLMSS). The results showed that considerably high hemicelluloses removal (94.57 %) and xylose yield (90.73 %) were achieved by the first step (CHTP, 160 °C, 1 h, 2 % of catalyst loading). The cascaded HADES treatment realized 90.25 % delignification ratio under the optimal conditions (120 °C, 3 h, 75 % of ADES loading), and the obtained residue could be easily converted into high-yield (93.35 %) of glucose via enzymatic saccharification. In addition, multiple enrichment cycle strategy (MECS) was performed to facilitate the recyclability of the HADES. The results showed that the enriched lignin recovered by MECS was activated by in-situ demethoxylation reaction. And such lignin fraction could be easily assembled into homogeneous lignin nanoparticles (LNPs, ∼31.51 nm in diameter) by simple sonication. Meanwhile, the MECS signally energized the antioxidant activity of the enriched lignin. Based on the high-efficiency cascade fractionation with the coupled CHTP-HADES fractionation strategy, it will observably boost the effectiveness and scalability of the advanced biorefinery strategy.