Mechanistic insights into the liquefaction stage of enzyme-mediated biomass deconstruction.

Effective enzyme-mediated viscosity reduction, disaggregation, or "liquefaction," is required to overcome the rheological challenges resulting from the fibrous, hygroscopic nature of lignocellulosic biomass, particularly at the high solids loadings that will be required for an economically viable process. However, the actual mechanisms involved in enzyme-mediated liquefaction, as determined by viscosity or yield stress reduction, have yet to be fully resolved. Particle fragmentation, interparticle interaction, material dilution, and water-retention capacity were compared for their ability to quantify enzyme-mediated liquefaction of model and more realistic pretreated biomass substrates. It was apparent that material dilution and particle fragmentation occurred simultaneously and that both mechanisms contributed to viscosity/yield stress reduction. However, their relative importance was dependent on the nature of the biomass substrate. Interparticle interaction and enzyme-mediated changes to these interactions was shown to have a significant effect on slurry rheology. Liquefaction was shown to result from the combined action of material dilution, particle fragmentation, and alteration of interactions at particle surfaces. However, the observed changes in water retention capacity did not correlate with yield stress reduction. The relative importance of each mechanism was significantly influenced by the nature of the biomass substrate and its physicochemical properties. An ongoing challenge is that mechanisms, such as refining, which enhance enzyme accessibility to the cellulosic component of the substrate, are detrimental to slurry rheology and will likely impede enzyme-mediated liquefaction when high substrate concentrations are used.

The use of carbohydrate binding modules (CBMs) to monitor changes in fragmentation and cellulose fiber surface morphology during cellulase- and Swollenin-induced deconstruction of lignocellulosic substrates.

Although the actions of many of the hydrolytic enzymes involved in cellulose hydrolysis are relatively well understood, the contributions that amorphogenesis-inducing proteins might contribute to cellulose deconstruction are still relatively undefined. Earlier work has shown that disruptive proteins, such as the non-hydrolytic non-oxidative protein Swollenin, can open up and disaggregate the less-ordered regions of lignocellulosic substrates. Within the cellulosic fraction, relatively disordered, amorphous regions known as dislocations are known to occur along the length of the fibers. It was postulated that Swollenin might act synergistically with hydrolytic enzymes to initiate biomass deconstruction within these dislocation regions. Carbohydrate binding modules (CBMs) that preferentially bind to cellulosic substructures were fluorescently labeled. They were imaged, using confocal microscopy, to assess the distribution of crystalline and amorphous cellulose at the fiber surface, as well as to track changes in surface morphology over the course of enzymatic hydrolysis and fiber fragmentation. Swollenin was shown to promote targeted disruption of the cellulosic structure at fiber dislocations.

Integrated acetic acid and deep eutectic solvent pretreatment on poplar for co-production of xylo-oligosaccharides, fermentable sugars and lignin antioxidants/adsorbents.

Efficient fractionation of lignocellulosic biomass in usable forms of hemicellulose, cellulose and lignin is very important for the sustainable lignocellulosic biorefinery. Herein, poplar sawdust was pretreated with an integrated process composed of acetic acid pre-hydrolysis (170 °C, 60 min) for xylo-oligosaccharides (XOS) production and mild deep eutectic solvent (90-130 °C, 60 min) post-delignification for recovering lignin fractions, resulting in easily hydrolyzed cellulose fraction. Results showed that, after integrated pretreatment and enzymatic hydrolysis, 51 % of xylan and 92 % of glucan in raw biomass could be converted to XOS (DP 2-6) and glucose, respectively, while 71 % of the original lignin could be recovered in DES solvent. The resulting XOS were proven to ensure the growth of probiotics, Bifidobacterium adolescentis. Besides, the lignin macromolecules recovered from DES solvent showed high-purity (around 95 %), low-molecular weight (Mw around 2000), small particle size (270-170 nm) and high-PhOH (3.08 mmol/g) content, which were likely relevant to the excellent antioxidant activity (RSI = 15.16) and adsorbent activity (Pb(II) 461.89 mg/g lignin). Finally, mass balance and energy analysis revealed that the integrated pretreatment could be used as a promising approach for the production of bio-based chemicals and materials from woody biomass.

Lignocellulosic biomass valorization via bio-photo/electro hybrid catalytic systems.

Lignocellulosic biomass valorization is regarded as a promising approach to alleviate energy crisis and achieve carbon neutrality. Bioactive enzymes have attracted great attention and been commonly applied for biomass valorization owing to their high selectivity and catalytic efficiency under environmentally benign reaction conditions. Same as biocatalysis, photo-/electro-catalysis also happens at mild conditions (i.e., near ambient temperature and pressure). Therefore, the combination of these different catalytic approaches to benefit from their resulting synergy is appealing. In such hybrid systems, harness of renewable energy from the photo-/electro-catalytic compartment can be combined with the unique selectivity of biocatalysts, therefore providing a more sustainable and greener approach to obtain fuels and value-added chemicals from biomass. In this review, we firstly introduce the pros/cons, classifications, and the applications of photo-/electro-enzyme coupled systems. Then we focus on the fundamentals and comprehensive applications of the most representative biomass-active enzymes including lytic polysaccharide monooxygenases (LPMOs), glucose oxidase (GOD)/dehydrogenase (GDH) and lignin peroxidase (LiP), together with other biomass-active enzymes in the photo-/electro- enzyme coupled systems. Finally, we propose current deficiencies and future perspectives of biomass-active enzymes to be applied in the hybrid catalytic systems for global biomass valorization.

Visible light laser direct-writing of high-resolution, biocompatible, super-multifunctional and tough hydrogels without photoinitiators in 30 s.

Currently, the lack of bioinks and long printing time limits the further development of biofabrication. Here we report a novel biocompatible, multi-functional and tough 3D printable hydrogel via visible light photocrosslinking of polyvinyl alcohol bearing styrylpyridinium group (PVA-SbQ). The high-resolution PVA-SbQ hydrogels with different designed shapes can be generated via laser direct-writing in 30 s without extra toxic crosslinkers or photoinitiators, and demonstrates excellent biocompatibility. The rapid laser direct-writing technology also results in a super-strong, tough hydrogel with excellent adhesive, swelling, self-healing, and photo-tunable properties due to the photodimerization of styrylpyridinium (SbQ) groups and the left-over massive amount of free hydroxyl groups in the hydrogel. For example, the maximum tensile strength, elongation, compressive strength adhesive strength of printed PVA-SbQ hydrogels can reach 1.0 MPa, 810 %, 33 MPa, 31 kPa, and 25,000 % respectively. And these properties can be adjusted by controlling the parameters for laser direct-writing. In addition, the introduced nitrogen cations by SbQ groups further endow hydrogels with the potential to develop novel functionality, which is demonstrated by integrating negatively charged nanocelluloses in the PVA-SbQ system to develop underwater adhesives, anti-freezing (-24.9 °C), and anti-bacterial hydrogels. This discovery opens multiple doors for developing PVA-SbQ based multi-functional hydrogel for various applications including biofabrication and tissue engineering.

Modified acid pretreatment to alter physicochemical properties of biomass for full cellulose/hemicellulose utilization.

Acid pretreatment of biomass decomposed hemicelluloses but could not effectively remove lignin, which hindered biomass saccharification and carbohydrates utilization. In this work, 2-naphthol-7-sulfonate (NS) and sodium bisulfite (SUL) were simultaneously added to acid pretreatment, which was found to synergistically increase hydrolysis yield of cellulose from 47.9 % to 90.6 %. Based on in-depth investigations, strong linear correlations were observed between cellulose accessibility and lignin removal, fiber swelling, CrI/cellulose ratio, cellulose crystallite size, respectively, indicating that some physicochemical characteristics of cellulose played significant roles in improving cellulose hydrolysis yield. After enzymatic hydrolysis, 84 % carbohydrates could be liberated and recovered as fermentable sugars for subsequent utilization. Mass balance illustrated that for 100 kg raw biomass, 15.1 kg xylonic acid and 20.5 kg ethanol could be co-produced, indicating the efficient utilization of biomass carbohydrates.

The coupling effects between acid-catalyzed hydrothermal pretreatment and acidic/alkaline deep eutectic solvent extraction for wheat straw fractionation.

Mild hydrothermal pretreatment (HP) integrating with solvent extraction is a promising two-step technique to enhance the overall lignin and carbohydrate output for lignocellulose fractionation. This work comparatively assessed the coupling effect between mild HP (the first step) and the emerging acidic choline chloride-natural acid or alkaline choline hydroxide based deep eutectic solvents (DES, the second step) for wheat straw fractionation. It was shown HP with 0.3% p-toluenesulfonic acid (p-TsOH) catalyst achieved a good compromise between complete hemicellulose removal (nearly 100%) and high cellulose recovery (99.2%). While choline hydroxide based DES showed better coupling effect with HP than choline chloride-natural acid DES, corresponding to 75.6 and 31.2% lignin removal respectively. It was proposed that the alkaline DES enhanced lignocellulose swelling the lignin phenolic hydroxyl groups deprotonation and thus facilitating lignin solubilization despite of its condensation at HP. Therefore, the alkaline DES resulting cellulose-rich fraction exhibited higher potential for further processing.

Surfactants facilitated glycerol organosolv pretreatment of lignocellulosic biomass by structural modification for co-production of fermentable sugars and highly reactive lignin.

This study reported that surfactants could facilitate the organosolv pretreatment of lignocellulosic biomass (LCB) to produce fermentable sugars and highly active lignin. Under the optimized conditions, the surfactant-assisted glycerol organosolv (saGO) pretreatment achieved 80.7% delignification with a retention of 93.4% cellulose and 83.0% hemicellulose. The saGO pretreated substrate exhibited an excellent enzymatic hydrolyzability, achieving 93% of glucose yield from the enzymatic hydrolysis at 48 h. Structural analysis showed that the saGO lignin contained rich ß-O-4 bondings with less repolymerization and lower phenolic hydroxyl groups, thus forming highly reactive lignin fragments. The analysis evidenced that the surfactant graft the lignin by structural modification, which was responsible for the excellent substrate hydrolyzability. The co-production of fermentable sugars and organosolv lignin almost recovered a gross energy (87.2%) from LCB. Overall, the saGO pretreatment holds a lot of promise for launching a novel pathway towards lignocellulosic fractionation and lignin valorization.

Towards efficient enzymatic saccharification of pretreated lignocellulose: Enzyme inhibition by lignin-derived phenolics and recent trends in mitigation strategies.

Lignocellulosic biorefinery based on sugar-platform has been considered as an efficient strategy to replace fossil fuel-based refinery. In the bioconversion process, pretreatment is an essential step to firstly open up lignocellulose cell wall structure and enhance the accessibility of carbohydrates to hydrolytic enzymes. However, various lignin and/or carbohydrates degradation products (e.g. phenolics, 5-hydroxymethylfurfural, furfural) are also generated during pretreatment, which severely inhibit the following enzymatic hydrolysis and the downstream fermentation process. Among them, the lignin derived phenolics have been considered as the most inhibitory compounds and their inhibitory effects are highly dependent on the source of biomass and the type of pretreatment strategy. Although liquid-solid separation and subsequent washing can remove the lignin derived phenolics and other inhibitors, this is undesirable in the realistic industrial application where the whole slurry of pretreated biomass needs to be directly used in the hydrolysis process. This review summarizes the phenolics formation mechanism for various commonly applied pretreatment methods and discusses the key factors that affect the inhibitory effect of phenolics on cellulose hydrolysis. In addition, the recent achievements on the rational design of inhibition mitigation strategies to boost cellulose hydrolysis for sugar-platform biorefinery are also introduced. This review also provides guidance for rationally designing detoxification strategies to facilitate whole slurry hydrolysis which helps to realize the industrialization of lignocellulose biorefinery.

Sustainable preparation of surface functionalized cellulose nanocrystals and their application for Pickering emulsions.

Herein, a highly efficient and sustainable approach, namely HCl-catalyzed para-toluene sulfonic acid/Formic acid (p-TsOH/FA) hydrolysis was reported to produce surface functionalized cellulose nanocrystals (CNCs). The optimized CNCs showed a high yield (79.6 %), high crystallinity (70.6 %) and high thermal stability (maximal weight loss temperature around 350 °C). In addition, the as-prepared CNCs possess excellent ability to stabilize oil-water due to the introduction of functional formyl groups, which could be promising stabilizers for Pickering emulsions (PEs). At a fixed oil-water ratio (2:8, v:v), the CNCs with the concentration of 0.5 wt% to 2.0 wt% could stabilize peanut oil to make PEs, and the emulsion droplets were <5 µm in diameter. In addition, the stability of the PEs at different temperature, pH, ionic strength, and long storage time were studied. The results indicated that the obtained CNCs could be sustainable and superior stabilizers for PEs.

A novel way to facilely degrade organic pollutants with the tail-gas derived from PHP (phosphoric acid plus hydrogen peroxide) pretreatment of lignocellulose.

The abundantly released tail-gas from lignocellulose pretreatment with phosphoric acid plus hydrogen peroxide (PHP) was found to accelerate the aging of latex/silicone textural accessories of the pretreatment device. Inspired by this, tail-gas was utilized to control organic pollutants. Methylene blue (MB), as a model pollutant, was rapidly decolorized by the tail-gas, and oxidative degradation was substantially proven by full-wavelength scanning with a UV-visible spectrometer. The tail-gas from six typical lignocellulosic feedstocks produced 68.0-98.3% MB degradation, suggesting its wide feedstock compatibility. Three other dyes, including rhodamine B, methyl orange and malachite green, obtained 97.5-99.5% degradation; moreover, tetracycline, resorcinol and hexachlorobenzene achieved 73.8-93.7% degradation, suggesting a superior pollutant compatibility. In a cytotoxicity assessment, the survival rate of the degraded MB was 103.5% compared with 80.4% for the untreated MB, implying almost no cytotoxicity after MB degradation. Mechanism investigations indicated that the self-exothermic reaction in PHP pretreatment drove the self-generated peroxy acids into tail-gas. Moreover, it heated the pollutant solution and thermally activated peroxy acids as free radicals for efficient pollutant degradation. Here, a brand-new technique for degrading organic pollutants with a "Win-Win-Win" concept was purposed for lignocellulose valorization, pollutant control by waste tail-gas, and biofuel production.

Insights into lignocellulosic waste fractionation for lignin nanospheres fabrication using acidic/alkaline deep eutectic solvents.

Facile fractionation of lignocellulosic waste into useable forms is essential to achieve a multi-product treatment process especially when the resulting lignin streams are expected for high-value materials valorization. Despite acidic/alkaline deep eutectic solvents (DESs) are promising solvents for lignocellulosic waste fractionation, there is little information about their differences in the fractionation and lignin extraction profiles. In this work, four DESs that were cataloged to acidic types (formic acid-choline chloride, lactic acid-choline chloride) and alkaline types (monoethanolamine-choline chloride, glycerol-K2CO3) were investigated to compare their abilities of bamboo waste fractionation. Physicochemical properties of these resulting cellulose, lignin and derived lignin nanospheres (LNPs) were also assessed. Results showed that DESs could selectively extract lignin via cleaving lignin-carbohydrate linkages and lignin ether bonds. Acidic DESs pretreatments were more effective in biomass delignification (~95.0 %), while alkaline DESs showed better polysaccharide retention. Glycerol-K2CO3 LNPs exhibited much smaller sphere size (50-100 nm) while acidic DESs LNPs showed higher thermal stability due to higher extent of lignin condensation. In addition, MEA-ChCl could introduce amine groups onto lignin hydroxyl. This work provided insightful information for tailoring technique routes to selective lignocellulosic waste fractionation, while facilitating the downstream applications of the obtained cellulose/lignin.

Why can hydrothermally pretreating lignocellulose in low severities improve anaerobic digestion performances?

A lignocellulosic residue, rice straw, was hydrothermally pretreated for the whole slurry anaerobic digestion. In contrast to the unpretreated rice straw, 110-120 °C pretreatment promoted biogas yield by 35%-38%, while only 14% promotion happened on the pretreatment at 180 °C. To understand why this improvement happened at lower severities, the pretreated rice straw at 90 °C, 120 °C, and 180 °C were selected for the further investigation, in which the liquor and solid fraction were separated for digestion, and compared with the whole slurry digestion. Results indicated more methane was released from the derived liquor of 180 °C than that of 90 °C and 120 °C, however, solid fraction did not exhibit significantly different methane yields (187.77-193.91 mL/g TS). These results suggested that the released soluble fraction from pretreatment could facilitate the methanogenesis. Furthermore, the released inherent soluble fraction in rice straw was mainly responsible for higher biogas yield at lower temperatures. Pretreatment at higher temperatures disintegrated the rice straw recalcitrance more, and intensified the release of soluble fraction accordingly. Consequently, the methanogenesis of whole slurry could be promoted at the initial digestion; the hydrolysis/acidification of the solid fraction in whole slurry was weakened greatly, which resulted in a lower biogas yield. This can also be proved by the evolution of dominant bacteria and archaea in the anaerobic digestion of whole slurry, separated solid and liquor fraction.

Bacterial cellulose/lignin nanoparticles composite films with retarded biodegradability.

In practical applications, the full biodegradability of all-biomass-based bacterial cellulose (BC) composites enhances their environmentally friendliness but results in the poor durability especially at humid conditions. This work prepared BC/lignin nanoparticles (LNPs) composite films with retarded biodegradability, which could broaden their application area. Three LNPs were fabricated using technical lignins extracted by deep eutectic solvent (DES), ethanol organosolv, soda/anthraquinone from poplar. LNPs involvement during BC fermentation showed limited influence on its productivity but significantly retarded the biodegradation of composite films. The potential inhibition mechanism was physical barrier and non-productive binding of LNPs. The BC/Soda LNPs showed much higher retarded degradation property (~58 wt% degradation) compared to BC/Organosolv LNPs and BC/DES LNPs (~85 wt% and ~ 97 wt% degradation respectively) at high enzyme loadings of 5 mg g-1 BCE. While at low enzyme loadings of 1 mg g-1 BCE, all these three composite films showed comparable retarded degradation property of ~60 wt%.

3-D hierarchical porous carbon from oxidized lignin by one-step activation for high-performance supercapacitor.

To convert lignin into high-valued carbon materials and understand the lignin structure function, oxidized lignin, a by-product from lignocellulose PHP-pretreatment (phosphoric acid plus hydrogen peroxide), was carbonized by one-step KOH-activation; the physico-chemical characteristics and electrochemical performances of the harvested carbons were also investigated. Results indicated the resultant carbons displayed 3-dimensional hierarchical porous morphology with maximum specific surface area of 3094 m2 g-1 and pore volume of 1.72 cm3 g-1 using 3:1 KOH/lignin ratio for carbonization. Three-electrode determination achieved a specific capacitance of 352.9 F g-1 at a current of 0.5 A g-1, suggesting a superior rate performance of this carbon. Two-electrode determination obtained an excellent energy density of 9.5 W h kg-1 at power density of 25.0 W kg-1. Moreover, 5000 cycles of charge/discharge reached 88.46% retention at 5 A g-1, implying an outstanding cycle stability. Basically, low molecular weight and abundant oxygen-containing functional groups of employed lignin mainly related to the excellent porous morphology and the outstanding electrochemical performances, suggesting the oxidized lignin was an ideal precursor to facilely prepare activated carbon for high-performance supercapacitor. Overall, this work provides a new path to valorize lignin by-product derived from oxidative pretreatment techniques, which can further promote the integrality of lignocellulose biorefinery.

n-p Heterojunction of TiO2-NiO core-shell structure for efficient hydrogen generation and lignin photoreforming.

Hydrogen evolution from biomass photoreforming has been widely recognized as a promising strategy for relieving the pressure from energy crisis and environmental pollution, as it could generate sustainable H2 and value-added bioproducts simultaneously. Combining p-type semiconductors with n-type semiconductors to form n-p heterojunction is an effective strategy to improve the photocatalytic quantum efficiency by enhancing the separation of photogenerated electrons and holes, which could greatly facilitate the realization of such biomass photorefinery concept. However, the incompact contact between the n-type and p-type semiconductors often induces the aggregation of photogenerated electrons and holes. In this work, we design and synthesize an ultrafine n-p heterojunction TiO2-NiO core-shell structure to overcome the incompact contact in the n-p interface. When the n-p heterojunction photocatalysts are evaluated for photocatalytic water splitting and biomass lignin photoreforming respectively, the as-fabricated TiO2-NiO nanocomposite with 3.25% NiO demonstrates the highest hydrogen generation of 23.5 mmol h-1 g-1 from water splitting and H2 (0.45 mmol h-1 g-1) and CH4 (0.03 mmol h-1 g-1) cogeneration with reasonable amount of fatty acids (palmitic acid and stearic acid) production from lignin photoreforming. The excellent photocatalytic activity is ascribed to the synergistic effects of high crystallinity of TiO2 ultrafine nanoparticles, core-shell structure and n-p heterojunction with NiO nanoclusters. This present work demonstrates a simple and efficient method to fabricate ultrafine n-p heterojunction core-shell structure for noble-metal free catalyst for both water splitting and biomass photoreforming.

Facile synthesis of manganese oxide modified lignin nanocomposites from lignocellulosic biorefinery wastes for dye removal.

In this study, a facile method to prepare MnO2 nanodots modified lignin nanocomposite (MnO2@LNP) was developed for efficient dye removal. The MnO2@LNP displayed hierarchical spherical nanostructures, where the MnO2 nanodots were evenly dispersed within the lignin nanosphere. Compared with lignin nanoparticles, the as-prepared MnO2@LNP exhibits higher surface area and can be separated after adsorption. It showed excellent adsorption capacity (806 mg/g) towards a typical cationic dye, methylene blue (MB), at a fast removal rate, where more than 80% of adsorption capacity was reached within 5 min at room temperature. The high adsorption capacity was contributed by the high surface area and negative charge on the adsorbent. The adsorption process is pH-responsive and exothermic, and the spent adsorbent can be reused for at least five cycles. This study displayed an efficient method to prepare MnO2@LNP for the high-value utilization of lignin-derived from lignocellulosic biorefinery.

Evaluation of Hydrothermal Pretreatment on Lignocellulose-Based Waste Furniture Boards for Enzymatic Hydrolysis.

Three typical waste furniture boards, including fiberboard, chipboard, and blockboard, were pretreated with conventional hydrothermal method. The responses of chemical composition, physicochemical morphology, and performances of enzymatic hydrolysis were evaluated. Results indicated the almost complete hemicellulose removal at higher pretreatment temperatures, the enhanced crystallinity index, and disordered morphology of the pretreated substrates indicated that the hydrothermal pretreatment deconstructed these boards well. However, the very low enzymatic hydrolysis (< 8% after 72 h) of the pretreated substrates showed the poor biological conversion. Three hypotheses for the weakened enzymatic hydrolysis were investigated, and results indicated that the residual adhesives and their degraded fractions were mainly responsible for poor hydrolysis. When NaOH post-pretreatment was attempted, cellulose-glucose conversion of the hydrothermally pretreated fiberboard, chipboard and blockboard can be improved to 28.5%, 24.1%, and 37.5%. Herein, the process of NaOH hydrothermal pretreatment was integrated, by which the hydrolysis of pretreated fiberboard, chipboard and blockboard was greatly promoted to 47.1%, 37.3%, and 53.8%, suggesting a possible way to pretreat these unconventional recalcitrant biomasses.

Fabrication of spherical lignin nanoparticles using acid-catalyzed condensed lignins.

Valorization of lignin by-products enhances the overall economics of current lignocellulose biorefinery. This work showed the high potential of fabricating acid-catalyzed condensed lignin fragments into high-value lignin nanoparticles (LNPs) with spherical structure. Four condensed lignins, i.e., liquid hot water pretreated hardwood aspen and eucalyptus lignin, steam pretreated softwood lodgepole pine and herbaceous corn stover lignin, were assessed for their abilities for LNPs using facile self-assembly method. Results showed the contents of condensed aromatics (0.20-0.67 mmol g-1) were varied with biomass species and hydrothermal pretreatment methods selected. Those resulting LNPs exhibited yields from 17.5 to 29.4%, particle sizes ranging from 20 to 100 nm and considerable suspension stabilities at pH 4-10. It was proposed that higher content of condensed lignin aromatics could provide more anchors available for their self-assembly through enhanced hydrophobic interactions, thus LNPs with more uniform particle size could be obtained. This work showed the technical opportunity to enhance the value of intractable condensed lignin through LNPs production towards a multi-product lignocellulose biorefinery.

Acidic deep eutectic solvents pretreatment for selective lignocellulosic biomass fractionation with enhanced cellulose reactivity.

This work tailored a promising two-step pretreatment, i.e., liquid hot water extraction followed by mild acidic deep eutectic solvents pretreatment for clean lignocellulose fractionation while enhancing cellulose reactivity for its subsequent utilization. The abilities of three acidic deep eutectic solvents (formic acid-, acetic acid- and lactic acid-choline chloride) to selectively extract poplar wood lignin and enhance cellulose reactivity were comparatively assessed. Results showed that rather high lignin selectivity of 6.3-7.9 was obtained while the available area and porosity of the resulting cellulose were significantly increased. The resulting cellulose pulps exhibited comparable chemical reactivity to commercial bleached Kraft pulp when cellulose acetate was selected as testing cellulose derivative for demonstrating purpose, showing their great promise for high-value use. It was proposed that the unique ionic properties of these acidic deep eutectic solvents were responsible for their selective lignin removal and cellulose swelling/deconstruction to enhance cellulose chemical reactivity.