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Utilization of three-dimensional biomass-derived porous carbons can effectively address issues of easy leakage, low thermal conductivity, and weak photothermal conversion of phase change materials (PCMs). This enables the production of high-performance composites for solar-induced energy collection, conversion, and storage. In this study, hierarchical lignin-derived porous carbon (HLPC), microporous lignin-derived porous carbon (MILPC) and mesoporous lignin-derived porous carbon (MELPC) were prepared through high-temperature in-situ activation using lignosulphonate (LS) as a carbon precursor and CaCO 3 , KOH and ZnCO 3 as activators. Carbon-based PCM composites with high performance were obtained by encapsulating paraffin wax (PW) in porous carbon supports. Results demonstrated that PW/HLPC exhibited comprehensive performance superior to other tested PW composites owing to its higher specific surface area (2,358 m 2 /g), larger pore volume (1.1 cm 3 /g) and well-interconnected framework structure. Additionally, PW/HLPC displayed relatively high latent heat (123.4 kJ/kg), photothermal conversion and storage efficiency (95 %), and photoelectric conversion performance (174.5 mV). Moreover, PW/HLPC also showed better leak-proof properties at 90 °C. The cycling stability and photothermal conversion performance of PW/HLPC were superior to those of the selected crude biochar-based PW composites. This study highlights the advantages of the prepared PW/HLPC for both the high-value utilization of lignin and its practical applications in solar-induced energy harvest, conversion, and storage., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

The cost of enzymolysis is a major bottleneck for the industrialisation of lignocellulosic enzymatic hydrolysis technology, and recycling cellulase can reduce this cost. Herein, a sulfobetaine prepolymer (CPS) with terminal chlorine was grafted onto enzymatic hydrolysis residual lignin (EHL) from corncob to construct thermosensitive lignin-based "molecular glues" (lignin-based sulfobetaine polymers, L-CPS) that were used to recover and recycle cellulase. L-CPS 2 (1.0 g/L) was added to the corncob residue (CCR) enzymolysis system (50 °C, pH 4.5). After hydrolysis, L-CPS 2 co-precipitated with cellulase through hydrophobic binding when cooling to 25 °C. This co-precipitation decreased the amount of cellulase by 40 %. In summary, a thermally responsive lignin-based molecular glue was constructed for green recycling of cellulase, providing a new approach to decreasing the cost of lignocellulosic enzymolysis and high value utilisation of industrial lignin., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Despite the widespread utilization of nano silver composites in the domain of catalytic hydrogenation of aromatic pollutants in wastewater, certain challenges persist, including the excessive consumption of chemical reagents during the preparation process and the difficulty in recycling. In this study, silver ions were reduced in-situ by taking advantage of the adsorptive and reducing capacities of hydroxyls and amino groups on lignin porous microspheres (LPMs) under mild ultrasonic conditions, and lignin porous microspheres loaded with silver nanoparticles (Ag@LPMs) were conveniently prepared. Ag@LPMs had excellent catalytic and cycling performances for p-nitrophenol (4-NP), methylene blue (MB) and methyl orange (MO). The 4-NP could be completely reduced to 4-AP within 155 s under the catalysis of Ag@LPMs, with a pseudo-first-order kinetic constant of 1.28 min -1 . Furthermore, Ag@LPMs could still complete the catalytic reduction of 4-NP within 10 min after five cycles. Ag@LPMs with the particle size ranging from 100 to 200 μm conferred ease of recycling, and the porous structure effectively resolved the issue of sluggish mass transfer encountered during the catalytic process. At the same time, the binding force of nano silver and LPMs obtained by ultrasonic was stronger than that of heating, so the materials prepared by ultrasonic had better cycling performance. Silver ions concentration and pH value in the preparation process affected the catalytic performance of Ag@LPMs, 50 mmol/L Ag + and pH value of 7 turned out to be the optimization conditions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper., (Copyright © 2024. Published by Elsevier B.V.)

Achieving superior photomineralization of pollutants relies on a rational design of a dual S-scheme with a robust internal electric field (IEF). In this study, to tackle the low mineralization rate in type-II In 2 O 3 /In 2 S 3 (IO/IS) systems, an organic-inorganic dual S-scheme In 2 O 3 /PDI/In 2 S 3 (IO/PDI/IS) nanostructured photocatalyst is synthesized via a method combining solvent-induced self-assembly and electrostatic forces. Due to the unique energy band position and strong IEF, the photoinduced defect-transit dual S-scheme IO/PDI/IS facilitates the degradation of lignin and antibiotics. Notably, a promising mineralization rate of 80.9% for sodium lignosulfonate (SL) is achieved. The charge transport pathway of IO/PDI/IS are further validated through the analysis of in situ X-ray photoelectron spectroscopy (in situ XPS), density functional theory calculations, and radical trapping experiments. In-depth, two possible pathways for the photocatalytic degradation of lignin are proposed based on the intermediates monitored by liquid chromatography-mass spectrometry (LC-MS). This study presents a new strategy for the design of organic-inorganic dual S-scheme photocatalysts with a robust IEF for pollutant degradation., (© 2023 Wiley-VCH GmbH.)

Thought-out utilization of entire lignocellulose is of great importance to achieving sustainable and cost-effective biorefineries. However, there is a trade-off between efficient carbohydrate utilization and lignin-to-chemical conversion yield. Here, we fractionate corn stover into a carbohydrate fraction with high enzymatic digestibility and reactive lignin with satisfactory catalytic depolymerization activity using a mild high-solid process with aqueous diethylamine (DEA). During the fractionation, in situ amination of lignin achieves extensive delignification, effective lignin stabilization, and dramatically reduced nonproductive adsorption of cellulase on the substrate. Furthermore, by designing a tandem fractionation-hydrogenolysis strategy, the dissolved lignin is depolymerized and aminated simultaneously to co-produce monophenolics and pyridine bases. The process represents the viable scheme of transforming real lignin into pyridine bases in high yield, resulting from the reactions between cleaved lignin side chains and amines. This work opens a promising approach to the efficient valorization of lignocellulose., (© 2024. The Author(s).)

In this study, a porous polyamine lignin microsphere (PPALM) was prepared through the inverse suspension polymerization combined with freeze-drying, during which sodium lignosulfonate and polyetheramine (PEA) were crosslinked with epichlorohydrin (ECH) as the cross-linker. By adjusting the amount of ECH and PEA, the optimized PPALM exhibited suitable crosslinking degree, ensuring a balance of framework flexibility and rigidity, thereby facilitating the formation of abundant and fine pores. PPALM demonstrated good mechanical properties comparable to commercial sulfonated polystyrene cationic resin, with a porosity of 61.12 % and an average pore size of 283.51 nm. The saturation adsorption capacity of PPALM for Pb 2+ was measured to be 156.82 mg/g, and it remained above 120 mg/g after five cycles of regeneration. Particularly, the concentration of 50 mg/L Pb 2+ solution could be reduced to 0.98 mg/L after flowing through the PPALM packed bed, indicating the great potential of PPALM for application in wastewater treatment., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have influenced the work reported in this paper., (Copyright © 2023. Published by Elsevier B.V.)

In situ integration of enzymes with covalent organic frameworks (COFs) to form hybrid biocatalysts is both significant and challenging. In this study, we present an innovative strategy employing deep eutectic solvents (DESs) to synergistically synthesize COFs and shield cytochrome c (Cyt c). By utilizing DESs as reaction solvents in combination with water, we successfully achieved rapid and in situ encapsulation of Cyt c within COFs (specifically COF-TAPT-TFB) under ambient conditions. The resulting Cyt c@COF-TAPT-TFB composite demonstrates a remarkable preservation of enzymatic activity. This encapsulation strategy also imparts exceptional resistance to organic solvents and exhibits impressive recycling stability. Additionally, the enhanced catalytic efficiency of Cyt c@COF-TAPT-TFB in a photoenzymatic cascade reaction is also showcased.

The enzymatic hydrolysis cost of lignocellulose can be reduced by improving enzymatic hydrolysis and recycling cellulase by adding additives. A series of copolymers P(SSS-co-SPE) (PSSPs) were synthesized using sodium p-styrene sulfonate (SSS) and sulfobetaine (SPE) as monomers. PSSP exhibited upper critical solution temperature response. PSSP with high molar ratio of SSS displayed more significant improved hydrolysis performance. When 10.0 g/L PSSP 5 was added to the hydrolysis system of corncob residues, and substrate enzymatic digestibility at 72 h (SED@72 h) increased by 1.4 times. PSSP with high molecular weight and moderate molar ratio of SSS, had significant temperature response, enhanced hydrolysis, and recovering cellulase properties. For high-solids hydrolysis of corncob residues, SED@48 h increased by 1.2 times with adding 4.0 g/L of PSSP 3 . Meanwhile, 50% of cellulase amount was saved at the room temperature. This work provides a new idea for reducing the hydrolysis cost of lignocellulose-based sugar platform technology., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Quantitatively understanding of interaction mechanism between lignin and cellulases is essential for the efficient improvement of lignocellulose enzymatic hydrolysis. However, the individual contribution of multiple forces between lignin and cellulases to the non-productive adsorption of enzymes still remains deeply ambiguous, especially in situations of near enzymatic hydrolysis temperatures. Herein, atomic force microscopy (AFM) and computational simulations were utilized to quantitatively analyze the intermolecular forces between lignin and enzyme at 25 °C and 40 °C. Our results unveiled that an increase in temperature obviously improved adsorption capacity and total intermolecular forces between lignin and cellulases. This positive relationship mainly comes from the increase in the decay length of hydrophobic forces for lignin-cellulases when temperature increases. Different from the hydrophobic interaction which provides long-range part of attractions, van der Waals forces dominate the intermolecular force only at approaches < 2 nm. On the other hand, electrostatic forces exhibited repulsive effects, and its intensity and distance were limited due to the low surface potential of cellulases. Short-range forces including hydrogen bonding (main) and π-π stacking (minor) stabilize the non-specific binding of enzymes to lignin, but increasing temperature reduces hydrogen bond number. Therefore, the relative contribution of long-range forces increased markedly at higher temperatures, which benefits protein capture and brings lignin and cellulase close together. Finally, the structure-activity relationships between lignin physicochemical properties and its inhibitory effect to enzymes indicated that hydrophobic interactions, hydrogen bonding, and steric effects drive the final adsorption capacity and glucose yields. This work provides quantitative and basic insights into the mechanism of lignin-cellulase interfacial interactions and guides design of saccharification enhancement approaches., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

Competing Interests: The authors declare no conflict of interest.

Heteroatom-doped porous carbon materials show promise for use as supercapacitor electrodes, but the tradeoff between surface area and the heteroatom dopant levels limits the supercapacitive performance. Here, we modulated the pore structure and surface dopants of N, S co-doped hierarchical porous lignin-derived carbon (NS-HPLC-K) via self-assembly assisted template-coupled activation. The ingenious assembly of lignin micelles and sulfomethylated melamine into a magnesium carbonate basic template greatly promoted the KOH activation process, which endowed the NS-HPLC-K with uniform distributions of activated N/S dopants and highly accessible nanosized pores. The optimized NS-HPLC-K exhibited a three-dimensional hierarchically porous architecture composed of wrinkled nanosheets and a high specific surface area of 2538.3 ± 9.5 m 2 /g with a rational N content of 3.19 ± 0.01 at.%, which boosted the electrical double-layer capacitance and pseudocapacitance. Consequently, the NS-HPLC-K supercapacitor electrode delivered a superior gravimetric capacitance of 393 F/g at 0.5 A/g. Furthermore, the assembled coin-type supercapacitor showed good energy-power characteristics and cycling stability. This work provides a novel idea for designing eco-friendly porous carbons for use in advanced supercapacitors., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

The cost of lignocellulosic enzymatic hydrolysis was reduced by enhancing enzymatic hydrolysis and recycling cellulase. Lignin-grafted quaternary ammonium phosphate (LQAP) with sensitive temperature and pH response, was obtained by grafting quaternary ammonium phosphate (QAP) onto enzymatic hydrolysis lignin (EHL). LQAP dissolved under the hydrolysis condition (pH 5.0, 50 °C) and enhanced the hydrolysis. After hydrolysis, LQAP and cellulase co-precipitated by the hydrophobic binding and electrostatic attraction, when lowering pH to 3.2, and cooling to 25 °C. LQAP had significant performances of pH-UCST response, enzymatic hydrolysis enhancement and cellulase recovery at the same time. When 3.0 g/L LQAP-100 was added to the system of corncob residue, SED@48 h increased from 62.6 % to 84.4 %, and 50 % of amount of cellulase was saved. Precipitation of LQAP at low temperature was mainly attributed to the salt formation of positive and negative ions in QAP; LQAP enhanced the hydrolysis for its ability to decrease the ineffective adsorption of cellulase by forming a hydration film on lignin and through the electrostatic repulsion. In this work, a lignin amphoteric surfactant with temperature response, was used to enhance hydrolysis and recover cellulase. This work will provide a new idea for reducing the cost of lignocellulose-based sugar platform technology, and high-value utilization of industrial lignin., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

The introduction of metal vacancies into n-type semiconductors could efficiently construct intimate contact interface p-n homojunctions to accelerate the separation of photogenerated carriers. In this work, a cationic surfactant occupancy method was developed to synthesize an indium-vacancy ( V In )-enriched p-n amorphous/crystal homojunction of indium sulfide (A/C-IS) for sodium lignosulfonate (SL) degradation. The amount of V In in the A/C-IS could be regulated by varying the content of added cetyltrimethylammonium bromide (CTAB). Meanwhile, the steric hindrance of CTAB produced mesopores and macropores, providing transfer channels for SL. The degradation rates of A/C-IS to SL were 8.3 and 20.9 times higher than those of crystalline In 2 S 3 and commercial photocatalyst (P25), respectively. The presence of unsaturated dangling bonds formed by V In reduced the formation energy of superoxide radicals ( • O 2 - ). In addition, the inner electric field between the intimate contact interface p-n A/C-IS promoted the migration of electron-hole pairs. A reasonable degradation pathway of SL by A/C-IS was proposed based on the above mechanism. Moreover, the proposed method could also be applicable for the preparation of p-n homojunctions with metal vacancies from other sulfides.

Photocatalytic water splitting to hydrogen is a sustainable energy conversion method. However, there is a lack of sufficiently accurate measurement methods for an apparent quantum yield (AQY) and a relative hydrogen production rate ( r H 2 ) at the moment. Thus, a more scientific and reliable evaluation method is highly required to allow the quantitative comparison of photocatalytic activity. Herein, a simplified kinetic model of photocatalytic hydrogen evolution was established, the corresponding photocatalytic kinetic equation was deduced, and a more accurate calculation method is proposed for the AQY and the maximum hydrogen production rate v H 2 ,max . At the same time, new physical quantities, absorption coefficient k L and specific activity SA, were proposed to sensitively characterize the catalytic activity. The scientificity and practicality of the proposed model and the physical quantities were systematically verified from the theoretical and experimental levels.

Metal-organic frameworks (MOFs) have become promising accommodation for enzyme immobilization in recent years. However, the microporous nature of MOFs affects the accessibility of large molecules, resulting in a significant decline in biocatalysis efficiency. Herein, a novel strategy is reported to construct macroporous MOFs by metal competitive coordination and oxidation with induced defect structure using a transition metal (Fe 2+ ) as a functional site. The feasibility of in situ encapsulating β-glucosidase (β-G) within the developed macroporous MOFs endows an enzyme complex (β-G@MOF-Fe) with remarkably enhanced synergistic catalysis ability. The 24 h hydrolysis rate of β-G@MOF-Fe (with respect to cellobiose) is as high as approximately 99.8%, almost 32.2 times that of free β-G (3.1%). Especially, the macromolecular cellulose conversion rate of β-G@MOF-Fe reached 90% at 64 h, while that of β-G@MOFs (most micropores) was only 50%. This improvement resulting from the expansion of pores (significantly increased at 50-100 nm) can provide enough space for the hosted biomacromolecules and accelerate the diffusion rate of reactants. Furthermore, unexpectedly, the constructed β-G@MOF-Fe showed a superior heat resistance of up to 120 °C, attributing to the new strong coordination bond (Fe 2+ -N) formation through the metal competitive coordination. Therefore, this study offers new insights to solve the problem of the high-temperature macromolecular substrate encountered in the actual reaction.

Organic pollutants pose a serious threat to water environment, thus it is essential to develop high-performance adsorbent to remove them from wastewater. Herein, nitrogen-doped magnetic porous carbon (M-PLAC) with three-dimensional porous structure was synthesized from lignin to adsorb methylene blue (MB) and tetracycline (TC) in wastewater. The calculated equilibrium adsorption amount by M-PLAC for MB and TC was 645.52 and 1306.00 mg/g, respectively. The adsorption of MB and TC on M-PLAC conformed to the pseudo-second-order kinetic model. The removal of MB by M-PLAC showed fast and efficient characteristics and exhibited high selectivity for TC in a binary system. In addition, M-PLAC was suitable for a variety of complex water environments and had good regeneration performance, demonstrating potential advantages in practical wastewater treatment. The organic pollutant adsorption by M-PLAC was attributed to electrostatic interaction, hole filling effect, hydrogen bonding, and the π-π interaction., (© 2022. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)

Recycling cellulase can reduce the cost of lignocellulosic enzymatic hydrolysis. Here, a lignin-grafted sulfobetaine (LSB) was first synthesized by grafting sulfobetaine (SB) on enzymatic hydrolysis lignin (EHL). LSB had a sensitive response of pH and temperature. LSB dissolved under the conditions of lignocellulosic enzymatic hydrolysis (pH 5.0, 50 °C). After hydrolysis, LSB co-precipitated with cellulase when lowering pH of the hydrolysate to 4.0 and cooling to 25 °C. When 3.0 g/L LSB-100 was added to the hydrolysis system of corncob residue (CCR), 70 % of amount of cellulase was saved. LSB had a remarkable response and stronger cellulase recovery capacity. This was attributed that carboxylate radical in LSB was protonated, and positive and negative ions of SB associated to form salt at 25 °C. This work provides a new idea for reducing the cost for preparing fermentable sugars from lignocellulose, and increasing the added value of EHL., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Due to the poor enzyme thermal stability, the efficient conversion of high crystallinity cellulose into glucose in aqueous phase over 50 °C is challenging. Herein, an enzyme-induced MOFs encapsulation of β-glucosidase (β-G) strategy was proposed for the first time. By using various methods, including SEM, XRD, XPS, NMR, FTIR and BET, the successful preparation of a porous channel-type flower-like enzyme complex (β-G@MOFs) was confirmed. The prepared enzyme complex (β-G@MOFs) materials showed improved thermal stability (from 50 °C to 100 °C in the aqueous phase) and excellent resistance to ionic liquids (the reaction temperature was as high as 110 °C) compared to the free enzyme (β-G). Not only the catalytic hydrolysis of cellulose by single enzyme (β-G) in ionic liquid was realized, but also the high-temperature continuous reaction performance of the enzyme was significantly improved. Benefiting from the significantly improved heat resistance, the β-G@MOFs exhibited 32.1 times and 34.2 times higher enzymatic hydrolysis rate compared to β-G for cellobiose and cellulose substrates, respectively. Besides, the catalytic activity of β-G@MOFs was retained up to 86 % after five cycles at 110 °C. This was remarkable because the fixation of the enzyme by the MOFs ensured that the folded structure of the enzyme would not expand at high temperatures, allowing the native conformation of the encapsulated protein well-maintained. Furthermore, we believe that this structural stability was caused by the confinement of flower-like porous MOFs., (© 2022 Wiley-VCH GmbH.)

Fast-response artificial phototropic materials are a promising tool for solar energy utilisation, yet their preparation remains challenging. Herein, we report the so-called photothermal domino strategy for constructing fast-response artificial phototropic materials. In this strategy, photothermal generation, heat conduction and thermal actuation are sequentially optimised by a coordination effect. For the first time, lignin-based organic radicals boosted by this coordination effect are used to significantly enhance photothermal conversion. Interfacial coordination bonds between lignin and an elastomer matrix promote interfacial heat conduction. Light-stimulated thermal actuation is significantly improved by coordination-assisted mechanical training. The prepared biomimetic phototropic material exhibits excellent phototropic ability, with a 2.5 s light-tracking process, showing great application potential for efficient solar energy utilisation. This strategy shows great significance for fabricating high-performance intelligent phototropic materials using widely available, green raw materials.

The photoreforming of lignocellulose is a novel method to produce clean and sustainable H 2 energy. However, the catalytic systems usually show low activity under ultraviolet light; thus, this reaction is very limited at present. Visible light-responsive metal-free two-dimensional graphite-phased carbon nitride (g-C 3 N 4 ) is a good candidate for photocatalytic hydrogen production, but its activity is hindered by a bulky architecture. Although reported layered g-C 3 N 4 modified with active functional groups prepared by the chemical exfoliation enhances the photocatalytic activity, it lost the intrinsic structure and thus is not conducive to understand the structure-activity relationship. Herein, we report an intrinsic monolayer g-C 3 N 4 (∼0.32 nm thickness) prepared by nitrogen-protected ball milling in water, which shows good performance of photoreforming lignocellulose to H 2 driven by visible light. The exciton binding energy of g-C 3 N 4 was estimated from the temperature-dependent photoluminescence spectra, which is a key factor for subsequent charge separation and energy transfer. It is found that monolayer g-C 3 N 4 with smaller exciton binding energy increases the free exciton concentrations and promotes the separation efficiency of charge carriers, thereby effectively improving its performance of photocatalytic reforming of lignocellulose, even the virgin lignocellulose and waste lignocellulose. This result could lead to more active catalysts to photoreform the raw biomass, making it possible to provide clean energy directly from locally unused biomass.

In this work, the coordination-based energy sacrificial bonds have been constructed in the interphase between lignin and polyolefin elastomer to prepare high performance lignin-based thermoplastic elastomers (TPEs). The strength and toughness of lignin-based TPEs can be adjusted by choosing different nitrogen heterocyclic compounds as reactive assistants and Fe 3+ or Zn 2+ as metal coordination centers. It was demonstrated that 3-Amino-1,2,4-triazole with three nitrogen atoms in the heterocyclic ring and one nitrogen branch chain could form the most efficient coordination bond system and generate the best mechanical performance. The system with ferric iron as coordination center exhibited better enhancement effect than divalent zinc. By adjusting the nitrogen-containing reactive additives or metal salts as coordination centers, the mechanical performance of the lignin-based TPE can be regulated, which provides a method for making green bio-composites with good strength and toughness, and also promotes the high value utilization of lignin in polymer materials., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Artificial muscle materials promise incredible applications in actuators, robotics and medical apparatus, yet the ability to mimic the full characteristics of skeletal muscles into synthetic materials remains a huge challenge. Herein, inspired by the dynamic sacrificial bonds in biomaterials and the self-strengthening of skeletal muscles by physical exercise, high performance artificial muscle material is prepared by rearrangement of sacrificial coordination bonds in the polyolefin elastomer via a repetitive mechanical training process. Biomass lignin is incorporated as a green reinforcer for the construction of interfacial coordination bonds. The prepared artificial muscle material exhibits high actuation strain (>40%), high actuation stress (1.5 MPa) which can lift more than 10,000 times its own weight with 30% strain, characteristics of excellent self-strengthening by mechanical training, strain-adaptive stiffening, and heat/electric programmable actuation performance. In this work, we show a facile strategy for the fabrication of intelligent materials using easily available raw materials.

Long-active conductivity, adhesiveness, and environmental stability are essential in the applications of hydrogel electronics. Integrating different functional materials into one system suffers from compatibility and cost problems. Inspired by the unique o-methoxyl structure in polyphenol lignin and its binding role in plants, catechol lignin (DAL) is constructed by one-step demethylation, which endows the lignin with a mussel-like bioadhesion, good reducibility, as well as a high ultraviolet absorption. The DAL is then applied to reduced graphene oxide, and the products-the oxidized DAL and the reduced graphene oxide mixture (DAL/rGO) is added into a sodium alginate/polyacrylamide (SA/PAM) double network hydrogel. Based on the Schiff base reaction between the quinone of the oxidized DAL and the amino of the skin, the DAL/rGO incorporated hydrogels could stably adhere to the skin, and sensitively respond to physiological signals. In addition, the DAL could provide the hydrogels with long-active sunscreen property when applied to real skin. These DAL based hydrogels have potential for on-skin sensing and outdoor sport equipment., (© 2021 Wiley-VCH GmbH.)

Green synthesis of silver nanoparticles (AgNPs) has received increasing attention. In this study, AgNPs were prepared through in-situ reduction by aminated alkaline lignin (AAL). Compared with alkaline lignin (AL), AAL exhibited stronger reduction capacity (increased by 36%) due to the introduced amine groups and better water solubility. Moreover, the coordination effect of amine groups on AAL improved the binding force between lignin and AgNPs. The content of AgNPs in AgNPs/AAL composite were 2.4 times higher than that in AgNPs/AL, such content could be further increased through increasing the reduction pH or prolonging the heating time. The results of XPS, XRD and TEM showed that the AgNPs were spherical and monodisperse with an average particle size about 17 nm. Additionally, the size of AgNPs was affected by the amination degree of lignin. AgNPs/AAL exhibited good catalytic performance for the reduction of 4-nitrophenol to 4-aminophenol, and this compound could be easily recovered and reused for at least eight cycles., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Inc. All rights reserved.)

This study reports on a comparative study of acid hydrotropic fractionation (AHF) of birch wood using maleic acid (MA) and p-toluenesulfonic acid (p-TsOH). Under the same level of delignification, lignin dissolved by MA is much less condensed with a higher content of ether aryl β-O-4 linkages. Lignin depolymerization dominated in MA hydrotropic fractionation (MAHF) and resulted in a single lower molecular weight peak, in contrast to the competitive depolymerization and repolymerization in p-TsOH AHF with a bimodal distribution. The less condensed MA-dissolved lignin facilitated catalytic conversion to monophenols. Carboxylation of residual lignin in fractionated cellulosic water-insoluble solids (WISs) enhanced enzymatic saccharification by decreasing nonproductive cellulase binding to lignin. At a low cellulase loading of 10 FPU g -1 glucan, saccharification of WIS-M T120 from MAHF at 120 °C was 95 % compared with 48 % for WIS-P T85 from p-TsOH AHF at 85 °C under the same level of delignification of 63 %. Residual lignin carboxylation also facilitated nanofibrillation of WIS for producing lignin-containing cellulose nanofibrils (LCNFs) through an enhanced lignin lubrication effect, which substantially decreases fibrillation energy. LCNFs from only one pass of microfluidization of WIS-M T120 have the same morphology as those from WIS-P T85 after three passes. MA also has a lower solubility and higher minimal hydrotropic concentration, which facilitated acid recovery. MA is U.S. Food and Drug Administration (FDA)-approved as an indirect food additive, affording significant advantages compared with p-TsOH for biorefinery applications., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Most additives that capable of enhancing enzymatic hydrolysis of lignocellulose are petroleum-based, which are not easy to recycle with poor biodegradability. In this work, highly recyclable and biodegradable sodium caseinate (SC) was used to enhance lignocellulosic hydrolysis with improved cellulase recyclability. When the pH decreased from 5.5 to 4.8, more than 96% SC could be precipitated from the solution and recovered. Adding SC increased enzymatic digestibility of dilute acid pretreated eucalyptus (Eu-DA) from 39.5% to 78.2% under Eu-DA loading of 10 wt% and pH = 5.5, and increase cellulase content in 72 h hydrolysate from only 15.2% of the original to 60.0%, which facilitated the recovery of cellulases through re-adsorption by fresh substrates. With multiple cycles of re-adsorption, application of SC not only increased the sugar yield of Eu-DA by 95.5%, but also reduced cellulase loading by 40%., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Oil-in-water (O/W) high internal phase emulsions (HIPEs) are widely used in foods, pharmaceuticals and cosmetics due to the high drug loading ratio, specific rheological behaviors and long shelf life. However, protective performance of active components within HIPEs maintains a low level. Herein, a series of carboxymethylated enzymatic hydrolysis lignin (EHL-CM-x) were synthesized by nucleophilic substitution and applied as macromolecular surfactant to stabilize the O/W HIPEs. It was found that EHL-CM-x combined with a small dosage of alkyl polyglycoside (APG) are able to stabilize HIPEs with 87 vol% soybean oil under neutral condition, which could be recognized as the highest internal phase reported in foods and pharmaceuticals. As a bioactive compound carrier, such EHL-CM-x stabilized HIPEs enable to provide outstanding UV, thermal and oxidation protection for sensitive natural extracts. The residual drug level obtained in this work is more than two times other gliadin/chitosan hybrid particles and sulfomethylated lignin stabilized HIPEs after UV irradiation. In vitro experiments showed that the minimum inhibitory concentration of curcumin within HIPEs against S. aureus and E. coli was 3.13 mg/mL and 12.5 mg/mL, respectively. Such lignin stabilized HIPEs could be potentially used in various areas, especially those with high stability and biosafety requirements., Competing Interests: Declaration of competing interest The authors declared that there is no conflict of interest., (Copyright © 2020 Elsevier B.V. All rights reserved.)

The isoelectric point (pI) of lignin-based surfactant is an important factor in the enhancement on the enzymatic hydrolysis of lignocellulose. In this work, lignin carboxylate (LC) and quaternary ammonium lignin carboxylates (LCQ-x, x%: the mass ratio of quaternizing agent to enzymatic hydrolysis lignin) with different isoelectric points were synthesized. LC or LCQ-x with pI significantly lower or higher than 4.8 reduced the non-productive adsorption of cellulase on lignin, but for the significant inhibitory effect on cellulase activity, their enhancements on the enzymatic hydrolysis of lignocellulose were not remarkable. However, LCQ-x with pI around 4.8 preserved the cellulase activity, and significantly reduced the non-productive adsorption of cellulase, therefore remarkably enhanced the enzymatic hydrolysis. 2 g/L LC, LCQ-40 (pI = 5.0) and LCQ-100 (pI = 9.2) increased the enzymatic digestibility of pretreated eucalyptus from 35.2% to 53.4%, 95.3% and 60.4% respectively. In addition, for the excellent pH-response performance, LCQ could be efficiently recovered after enzymatic saccharification., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

A lignin amphoteric surfactant and betaine could enhance the enzymatic hydrolysis of lignocellulose and recover cellulase. The effects of lignosulfonate quaternary ammonium salt (SLQA) and dodecyl dimethyl betaine (BS12) on enzymatic hydrolysis digestibility, ethanol yield, yeast cell viability, and other properties of high-solid enzymatic hydrolysis and fermentation of a corncob residue were studied in this research. The results suggested that SLQA and 1 g/L BS12 effectively improved the ethanol yield through enhancing enzymatic hydrolysis. SLQA had no significant effect on the yeast cell membrane and glucose fermentation. However, 5 g/L BS12 reduced the ethanol yield as a result of the fact that 5 g/L BS12 damaged the yeast cell membrane and inhibited the conversion of glucose to ethanol. Our research also suggested that 1 g/L BS12 enhanced the ethanol yield of corncob residue fermentation, which was attributed to the fact that lignin in the corncob adsorbed BS12 and decreased its concentration in solution to a safe level for the yeast.

The origin, amount, hydrophilicity, charge, molecular weight and its distribution of lignin have significant influences on the enzymatic hydrolysis of lignocellulose. The enzymatic hydrolysis of lignocellulose was essentially enhanced by lignin-based polyoxyethylene ether (EHL-PEG), whereafter followed by PEG4600 and lignosulfonate (LS). The effect of LS, EHL-PEG and PEG4600 on the adsorption and enzymatic hydrolysis kinetics of cellulase on the gold surface and cellulose film was investigated by Quartz Crystal Microbalance with dissipation monitoring (QCM-D). Results showed that the interaction of LS or EHL-PEG with cellulase was electrostatic attractive and hydrophobic effect, respectively, and formed hydrophilic cellulase aggregates. LS-Cellulase peeled off the cellulose film layer by layer, while the hydrophobic phenylpropane structure of EHL-PEG-Cellulase acted as a cellulose binding domain to hydrolysis cellulose through "Hollow" effect and made cellulose become more loose and swollen. At last, a strategy to enhance the enzymatic hydrolysis of lignocellulose by lignin-based amphiphilic polymers was proposed as well., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

In this work, a novel star-comb copolymer based on poly(d,l-lactide) (PDLLA) macromonomer and poly(ethylene glycol)methyl ether methacrylate (PEGMA) was prepared, and the electrochemical properties were studied, with the aim of using it as a solid polymer electrolyte in lithium ion batteries. The six-arm vinyl functionalized PDLLA macromonomer was synthesized by a ring-opening polymerization (ROP) of d,l-lactide and subsequently an acylation of the hydroxy end-groups. A series of free-standing solid polymer electrolyte membranes from different ratios of PDLLA, PEGMA and LiTFSI were prepared through solvent-free free radical polymerization under UV radiation. The chemical structure of the obtained polymers was confirmed by 1 H NMR and FTIR. The as-prepared six-arm star-comb solid polymer electrolytes (PDLLA-SPEs) exhibit good thermal stability with T d 5% s of ∼270 °C and low T g s of -48 to -34 °C. The electrochemical characterization shows that the PDLLA-SPEs possess a wide electrochemical window up to 5.1 V with an optimal ionic conductivity of 9.7 × 10 -5 S cm -1 at 60 °C at an EO/Li + ratio of 16 : 1. Furthermore, the all-solid-state LiFePO 4 /Li cells display extraordinary cycling and rate performances at 60 °C by curing the PDLLA-SPEs directly on the cathode. These superior properties of the six-arm star-comb PDLLA-SPE make it a promising candidate solid electrolyte for lithium batteries., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Effects of nonionic surfactants on enzymatic hydrolysis of Avicel at different agitation rates and solid loadings and the mechanism were studied. Nonionic surfactants couldn't improve the enzymatic hydrolysis efficiency at 0 and 100rpm but could enhance the enzymatic hydrolysis significantly at high agitation rate (200 and 250rpm). Cellulase was easily deactivated at high agitation rate and the addition of nonionic surfactants can protect against the shear-induced deactivation, especially when the cellulase concentration was low. When 25mg protein/L of cellulase solution was incubated at 200rpm for 72h, the enzyme activity increased from 36.0% to 89.5% by adding PEG4600. Moreover nonionic surfactants can compete with enzyme in air-liquid interface and reduce the amount of enzyme exposed in the air-liquid interface. The mechanism was proposed that nonionic surfactants could enhance the enzymatic hydrolysis of Avicel by reducing the cellulase deactivation caused by shear force and air-liquid interface., (Copyright © 2017. Published by Elsevier Ltd.)

Triblock copolymer polydopamine-polyacrylic-polyoxyethylene (PDA-PAA-PEO) with excellent performance as a binder for silicon anodes was synthesized. Its structure was confirmed by 1 H-NMR, FTIR and UV-vis spectroscopy. Results of electrochemical measurements indicated that a silicon anode based on PDA-PAA-PEO binder exhibited excellent cycle performance with a reversible capacity of 1597 mA h g -1 after 200 cycles at a current density of 0.5 C, much better than that of an electrode based on a polyvinylidene-fluoride binder. Improvement of the cycle performance and reversible capacity for silicon anodes could be attributed to the strong adhesive and high ion conductivity of PDA-PAA-PEO., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)

Lignin is a vastly underutilized biomass resource. The preparation of water-dispersed lignin nanoparticles is an effective way to realize the high-value utilization of lignin. However, the currently reported preparation methods of lignin nanoparticles still have some drawbacks, such as the requirement for toxic organic solvent or chemical modification, complicated operation process, and poor dispersibility. Here, lignin/sodium dodecyl sulfate (SDS) composite nanoparticles (LSNPs) with outstanding water dispersibility and a size range of 70-200 nm were facilely prepared via acidifying the mixed basic solution of alkaline lignin and SDS. No harsh chemical was needed. The formation mechanism was systematically studied. Results indicated that the LSNPs were obtained by acid precipitation of the mixed micelles formed by the self-assembly of lignin and SDS. In addition, on the basis of the LSNP-stabilized Pickering emulsions, lignin/polyurea composite microcapsules combining the excellent chemical stability of a synthetic polyurea shell with the fantastic antiphotolysis and antioxidant properties of lignin were successfully prepared.

Some zwitterionic surfactants exhibit upper critical solution temperature (UCST) in aqueous solutions. For the zwitterionic surfactant solution mixed with cellulase, when its temperature is below UCST, the cellulase can be recovered by coprecipitation with zwitterionic surfactant. In this work, 3-(Hexadecyldimethylammonio) propanesulfonate (SB3-16) was selected to enhance the enzymatic hydrolysis of lignocelluloses and recover the cellulase. After adding 2mmol/L of SB3-16, the enzymatic digestibility of eucalyptus pretreated by dilute acid (Eu-DA) and by sulfite (Eu-SPORL) increased from 27.9% and 35.1% to 72.6% and 89.7%, respectively. The results showed that SB3-16 could reduce the non-productive adsorption of cellulase on hydrophobic interface, while it did not significantly inhibit the activity of cellulase. For the solution contained 1wt% SB3-16 and 200mg protein/L CTec2 cellulase, 55.2% of protein could be recovered by cooling. The filter paper activity of the recovered cellulase was 1.93FPU/mg protein, which was 95.8% of its initial activity., (Copyright © 2017. Published by Elsevier Ltd.)

Polyvinylpyrrolidone (PVP) is an antifouling polymer to resist the adsorption of protein on solid surface. Effects of PVP on the enzymatic hydrolysis of pretreated lignocelluloses and its mechanism were studied. Adding 1g/L of PVP8000, the enzymatic digestibility of eucalyptus pretreated by dilute acid (Eu-DA) was increased from 28.9% to 73.4%, which is stronger than the classic additives, such as PEG, Tween and bovine serum albumin. Compared with PEG4600, the adsorption of PVP8000 on lignin was larger, and the adsorption layer was more stable and hydrophilic. Therefore, PVP8000 reduced 73.1% of the cellulase non-productive adsorption on lignin and enhanced the enzymatic hydrolysis of lignocelluloses greatly., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Two pretreatment methods to overcome recalcitrance of lignocelluloses, sulfite pretreatment (SPORL) and dilute acid (DA), were conducted to pretreat softwood masson pine and hardwood eucalyptus for enzymatic hydrolysis. In the presence of corresponding pre-hydrolysates, adding moderate cetyltrimethylammonium bromide (CTAB) could enhance the enzymatic hydrolysis of the SPORL-pretreated substrates, but had no enhancement for the DA-pretreated substrates. The results showed that sodium lignosulfonate (SL) in pre-hydrolysates and CTAB together had a strong enhancement on the enzymatic hydrolysis of lignocelluloses. The compound of commercial lignosulfonate SXSL and CTAB (SXSL-CTAB) could enhance the substrate enzymatic digestibility (SED) of SPORL-pretreated masson pine from 27.1% to 71.0%, and that of DA-pretreated eucalyptus from 37.6% to 67.9%. The mechanism that CTAB increased the adsorption of SL on lignin to form more effective steric hindrance and reduced the non-productive adsorption of cellulase on lignin by neutralizing the negative charge of SL was proposed., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Unlabelled: Sulfonated-acetone-formaldehyde (SAF) was grafted with alkali lignin (AL) to prepare grafted sulfonated-acetone-formaldehyde lignin (GSL). Considering the rich phenolic hydroxyl groups in GSL, we detected a hole mobility of 2.27 × 10(-6) cm(2) V(-1) s(-1) with GSL as a hole transport material by space-charge-limited current model. Compared with nonconjugated poly(styrene sulfonic acid), GSL was applied as p-type semiconductive dopant for PEDOT to prepare water-dispersed, Pedot: GSL., Pedot: GSL shows enhanced conductivity compared with that of, Pedot: PSS. Simultaneously, the enhanced open-circuit voltage, short-circuit current density, and fill factor are achieved using, Pedot: GSL as a hole extract layer (HEL) in sandwich-structure inverted perovskite solar cells. The power conversion efficiency is increased to 14.94% compared with 12.6% of, Pedot: PSS-based devices. Our results show that amorphous GSL is a good candidate as dopant of PEDOT, and we provide a novel prospective for the design of HEL based on lignin, a renewable biomass and phenol derivatives.

Sodium lignosulfonate (SXSL) and long-chain fatty alcohols (LFAs) could enhance the enzymatic hydrolysis of xylan, and the compound of SXSL and LFAs have synergies on the enzymatic hydrolysis. SXSL shows a strong enhancement in buffer pH range from 4.0 to 6.0. The enhancement increased with the SXSL dosage and the xylanase loading. The cellulose and lignin in corncob substrate could not only adsorb xylanase nonproductively, but also seriously reduce the accessibility of xylanase on xylan to impede the enzymatic hydrolysis of xylan. Cellulase could break the plant cell wall structure of corncob and make additives work better. The xylose yield of corncob at 72h increased from 59.4% to 73.7% by adding the compound of 5g/L SXSL and 0.01% (v/v) n-decanol, which was higher than that without cellulase and additives by 30.7%. Meanwhile, the glucose yield at 72h of corncob increased from 45.8% to 62.3%., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Effect of the molecular structure of lignin-based polyoxyethylene ether (EHL-PEG) on enzymatic hydrolysis of Avicel and corn stover was investigated. With the increase of PEG contents and molecular weight of EHL-PEG, glucose yield of corn stover increased. EHL-PEG enhanced enzymatic hydrolysis of corn stover significantly at buffer pH 4.8-5.5. Glucose yield of corn stover at 20% solid content increased from 32.8% to 63.8% by adding EHL-PEG, while that with PEG4600 was 54.2%. Effect of EHL-PEG on enzymatic hydrolysis kinetics of cellulose film was studied by quartz crystal microbalance with dissipation monitoring (QCM-D) and atomic force microscopy (AFM). An enhancing mechanism of EHL-PEG on enzymatic hydrolysis kinetics of cellulose was proposed. Cellulase aggregates dispersed by EHL-PEG excavated extensive cavities into the surface of cellulose film, making the film become more loose and exposed. After the maximum enzymatic hydrolysis rate, the film was mainly peeled off layer by layer until equilibrium., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Water-soluble lignin-based polyoxyethylene ether (EHL-PEG), prepared from enzymatic hydrolysis lignin (EHL) and polyethylene glycol (PEG1000), was used to improve enzymatic hydrolysis efficiency of corn stover. The glucose yield of corn stover at 72h was increased from 16.7% to 70.1% by EHL-PEG, while increase in yield with PEG4600 alone was 52.3%. With the increase of lignin content, EHL-PEG improved enzymatic hydrolysis of microcrystalline cellulose more obvious than PEG4600. EHL-PEG could reduce at least 88% of the adsorption of cellulase on the lignin film measured by quartz crystal microbalance with dissipation monitoring (QCM-D), while reduction with PEG4600 was 43%. Cellulase aggregated at 1220nm in acetate buffer analyzed by dynamic light scattering. EHL-PEG dispersed cellulase aggregates and formed smaller aggregates with cellulase, thereby, reduced significantly nonproductive adsorption of cellulase on lignin and enhanced enzymatic hydrolysis of lignocelluloses., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

The effects of lignosulfonate (SXSL) and long-chain fatty alcohols (LFAs) on the rheology and enzymatic hydrolysis of high-solid corncob slurries were investigated. The application of 2.5% (w/w) SXSL increased the substrate enzymatic digestibility (SED) of high-solid corncob slurries at 72 h from 31.7 to 54.0%, but meanwhile it increased the slurry's yield stress and complex viscosity to make the slurry difficult to stir and pump. The smallest molecular weight (MW) SXSL fraction had the strongest enhancement on SED. The SXSL fraction with large MW had a negative effect on rheology. n-Octanol (C8) and n-decanol (C10) improved the rheological properties of high-solid slurry and are strong enough to counteract the negative effect of SXSL. Furthermore, C8 and C10 clearly enhanced the enzymatic hydrolysis of high-solid corncob slurries with and without SXSL. A mechanism was proposed to explain the observed negative effect of SXSL and the positive effect of LFAs on the rheological properties.

Alkali lignin (AL) was employed as raw materials in the present study. Sulfomethylation was conducted to improve the solubility of AL, while sulfomethylated alkali lignin (SAL) was further polymerized by horseradish peroxidase (HRP). HRP modification caused a significant increase in molecular weight of SAL which was over 20 times. It was also found to increase the amount of sulfonic and carboxyl groups while decrease the amount of phenolic and methoxyl groups in SAL. The adsorption quantity of self-assembled SAL film was improved after HRP modification. Sulfonation and HRP modification were mutually promoted. The polymerization reactivity of SAL in HRP modification was increased with its sulfonation degree. Meanwhile, HRP modification facilitated SAL's radical-sulfonation reaction., (Copyright © 2014. Published by Elsevier Ltd.)

Four fractions of one commercial sodium lignosulfonate (SXP) with different molecular weight (MW) and anionic polymers were studied to reduce non-productive adsorption of cellulase on bound lignin in a lignocellulosic substrate. SXP with higher MW had stronger blocking effect on non-productive adsorption of a commercial Trichoderma reesi cellulase cocktail (CTec2) on lignin measured by quartz crystal microgravimetry with dissipation monitoring. Linear anionic aromatic polymers have strong blocking effect, but they would also reduce CTec2 adsorption on cellulose to decrease the enzymatic activity. The copolymer of lignin and polyethylene glycol (AL-PEG1000) has strong enhancement in enzymatic hydrolysis of lignocelluloses, because it not only improves the cellulase activity to cellulose, but also blocks the non-productive cellulase adsorption on lignin. Apart from improving the cellulase activity to cellulose, the enhancements of enzymatic hydrolysis of lignocellulose by adding AL-PEG1000 and SXPs are the result of the decreased cellulase non-productive adsorption on lignin., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

We studied the mechanism of the significant enhancement in the enzymatic saccharification of lignocelluloses at an elevated pH of 5.5-6.0. Four lignin residues with different sulfonic acid contents were isolated from enzymatic hydrolysis of lodgepole pine pretreated by either dilute acid (DA) or sulfite pretreatment to overcome recalcitrance of lignocelluloses (SPORL). The adsorption isotherms of a commercial Trichoderma reesi cellulase cocktail (CTec2) produced by these lignin residues at 50 °C were measured in the pH range of 4.5-6.0. The zeta potentials of these lignin samples were also measured. We discovered that an elevated pH significantly increased the lignin surface charge (negative), which causes lignin to become more hydrophilic and reduces its coordination affinity to cellulase and, consequently, the nonspecific binding of cellulase. The decreased nonspecific cellulase binding to lignin is also attributed to enhanced electrostatic interactions at elevated pH through the increased negative charges of cellulase enzymes with low pI. The results validate the hypothesis that the increases in enzymatic saccharification efficiencies at elevated pH for different pretreated lignocelluloses are solely the result of decreased nonspecific cellulase binding to lignin. This study contradicts the well-established concept that the optimal pH is 4.8-5.0 for enzymatic hydrolysis using Trichoderma reesi cellulose, which is widely accepted and exclusively practiced in numerous laboratories throughout the world. Because an elevated pH can be easily implemented commercially without capital cost and with minimal operating cost, this study has both scientific importance and practical significance., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)