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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Synthesis of Highly Strained Cyclobutane Fuels via Room-Temperature-Integrated Oxidation/[2 + 2] Cycloaddition of Lignocellulose-Based Cyclic Ketones and Cyclic Alcohols

Jun Zhang,Xiu-tian-feng E,Bo Yang,Xiumei Ma,Xueping Wang,Ninghui Chang,Qiuyu Zhang,Ji-Jun Zou,Junjian Xie

High-energy-density cyclobutane fuels were directly synthesized via room-temperature-integrated one-pot two-step oxidation/self-photosensitized [2 + 2] cycloaddition using lignocellulose-derived cyclic ketones and cyclic alcohols for the first time, which endow much higher density, lower freezing point, and higher neat heat of combustion than other biofuels achieved from the same feedstocks and hence denote a new kind of sustainable high-density fuels appealing for practical applications.

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INDUSTRIAL CROPS AND PRODUCTS · 2025 · IF 6.2

Highly efficient conversion of cellulose and hemicellulose using an innovative ternary deep eutectic solvent: Achieving the green and complete use of lignocellulose

Jianxun Ma,Nyuk Ling Ma,Wenqi Zhang,Yu Wu,Yue Ma,Guang Chen,Yang Sun,Jihong Wang,Chunyu Sun

Efficient pretreatment plays a key role in enhancing lignocellulose resources utilization. This study introduces a novel lignocellulose conversion approach using a newly developed ternary deep eutectic solvents (DES) consisting of Choline Chloride, Urea, and Ethylenediamine (ChCl-U-EDA 1:1.4:0.6). The enzymatic efficiencies of cellulase and hemicellulase reached 90.99 % and 76.77 %, respectively. Under the condition of 110 °C, 90 min, and a 1:15 solid to liquid ratio, the enzymatic hydrolysis of DES-pretreated lignocellulose yielded glucose and xylose at 0.52 g/g and 0.21 g/g, respectively. The lignin isolated from ChCl-U-EDA pretreatment displayed a more preserved structure with enhanced retention of β-O-4 bonds. Reduced density gradient analysis and molecular dynamics simulation indicated that the hydrogen bonding between lignin and ChCl-U-EDA facilitates the detachment of lignin from lignocellulose. The extracted lignin was then fabricated into a hydrogel for yeast immobilization, facilitating bioethanol production from glucose and xylose. After ten cycles, the average sugar to ethanol conversion was 0.448 g/g, corresponding to 89.6 % sugar conversion to ethanol. Reuse of ChCl-U-EDA resulted in 62.13 % lignin collection after 5 cycles. This study proposes a novel approach for the comprehensive and sustainable conversion of lignocellulose in an environmentally friendly and efficient manner.

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Arabian Journal of Chemistry · 2022 · IF 6.212

Exploring the promoting mechanisms of bovine serum albumin, lignosulfonate, and polyethylene glycol for lignocellulose saccharification from perspective of molecular interactions with cellulase

Peipei Wang,Qingcheng Wang,Tian Liu,Jiaqi Guo,Yongcan Jin,Huining Xiao,Junlong Song

Bovine serum albumin (BSA), polyethylene glycol (PEG) and lignosulfonate (LS) have been extensively employed as synergistic agents in lignocellulose saccharification. Nevertheless, the promoting mechanisms have not been fully understood and there are a number of controversial opinions existed. All attention has been paid to the interactions between respective additive and substrate. However, rarely attention has been paid to the interactions between additives and enzymes (cellulase from Trichoderma reesei in this investigation). This interaction is actually more important since cellulase interacts with the additives before it contacts with substrate. Therein, Quartz crystal microbalance with dissipation monitoring (QCM-D), surface plasma resonance (SPR) and small angel X-ray scattering (SAXS) were incorporated to study the interaction between enzyme and additives. The results showed synergistic agents have different interaction modes with cellulase. BSA and LS can form complexes with cellulase and the formed complexes prevent them from nonproductive binding by residue lignin; what’s more, the cellulase-BSA complexes improve the hydrolytic capability of pristine enzyme whereas cellulase-LS complexes reduce. PEG prevents the unproductive binding of cellulase to the residual lignin by forming a thin layer that actually acts as a steric hindrance to the residual lignin. This investigation helps us to understand the sophisticated interactions among the components in the complicated enzymatic system, especially the interactions between enzymes and synergistic agents. It will be helpful in the design and utilization of synergistic additives in the lignocellulose biorefinery process as well.

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BIORESOURCE TECHNOLOGY · 2015 · IF 4.494

Fast microwave-assisted preparation of a low-cost and recyclable carboxyl modified lignocellulose-biomass jute fiber for enhanced heavy metal removal from water

Zhaolin Du,Tong Zheng,Peng Wang,Linlin Hao,Yanxia Wang

A low-cost and recyclable biosorbent derived from jute fiber was developed for high efficient adsorption of Pb(II), Cd(II) and Cu(II) from water. The jute fiber was rapidly pretreated and grafted with metal binding groups ( COOH) under microwave heating (MH). The adsorption behavior of carboxyl-modified jute fiber under MH treatment (CMJF MH ) toward heavy metal ions followed Langmuir isotherm model ( R 2   >   0.99) with remarkably high adsorption capacity (157.21, 88.98 and 43.98   mg/g for Pb(II), Cd(II) and Cu(II), respectively). Also, CMJF MH showed fast removal ability for heavy metals in a highly significant correlation with pseudo second-order kinetics model. Besides, CMJF MH can be easily regenerated with EDTA-2Na solution and reused up to at least four times with equivalent high adsorption capacity. Overall, cheap and abundant production, rapid and facile preparation, fast and efficient adsorption of heavy metals and high regeneration ability can make the CMJF MH a preferred biosorbent for heavy metal removal from water.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

A practical regeneration approach and model simulation for poisoned-resin recycle to selectively detoxify acetic acid-like bio-inhibitors in acidic lignocellulose hydrolysate

Jian Han,Danfeng Li,Feng Han,Kaijian Huang,Fuyu Yang,Yong Xu

Selective removal of degradation inhibitors from lignocellulosic biorefinery with resins is a very effective and easy operation. However, the resin will be heavily contaminated after the detoxification. The regeneration and recycle of poisoned-resin are difficult but necessary to overcome commercial production cost. In this study, various methods were compared to regenerate the poisoned-resin and finally 5% H 2 O 2 for 5 h and 1 M NaOH for 4 h were chosen. This combined technology can recover the adsorption efficiency of regenerated resin to 86.97 % and 80.49 % for bio-inhibitors. The Boyd model and the Van't Hoff equation were used to fit the kinetics and thermodynamics of the regeneration process, respectively. The poisoned-resin maintained more than 63.3 % adsorption efficiency to acetic acid after three regeneration cycles and adsorbed fewer sugars. Even using several cycles of regenerated resin to detoxify the crude acidic hydrolysate, the biocatalytic performance of xylose to xylonic acid was increased from 18.6 % to 44.6 %. Moreover, the alkali can be recycled during the regeneration process, which can avoid the use of large amounts of alkali. This work could provide a green and practical approach for poisoned-resin recycle, and especially promote the technological development of lignocellulosic hydrolysate fermentation.

研究领域: 生物工程 · 环境科学
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

LED white-light-driven photocatalysis for effective lignocellulose reforming to co-produce hydrogen and value-added chemicals via Zn2/O@IP-g-CN

Jiliang Ma,Junqiang Zhang,Dongnv Jin,Shuangquan Yao,Runcang Sun

Synchronous photocatalytic water splitting and the reforming of a biomass-derived feedstock to generate hydrogen and high-value-added chemicals make full utilization of the biomass-water-splitting redox reaction; however, limited successes in this regard have been reported. Herein, incompletely polymerized graphitic carbon nitride co-doped with zinc/oxygen atoms (Zn 2 /O@IP- g -CN) was prepared via a step-by-step low-temperature calcination process with the assistance of melamine and zinc phthalocyanine, which successfully resulted in simultaneous photocatalytic water splitting and the reforming of biomass-derived monosaccharides to produce hydrogen (11436.7 μmol g −1 h −1 ) and lactic acid (92.6 %), respectively. Zn 2 /O@IP- g -CN exhibits a fast separation/migration rate and low resistance compared to those of pure CN, resulting in Zn 2 /O@IP- g -CN showing enhanced photocatalytic activity. The hydrogen release rate of 86.8 % and lactic acid yield of 89.0 % were retained compared to initial values when Zn 2 /O@IP- g -CN was reused in 5 th cycles. Poisoning experiments indicated that 1 O 2 , ·O 2 - , ·OH, and h + were all beneficial for lactic acid production.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2021 · IF 6.953

Lignocellulose-based free-standing hybrid electrode with natural vessels-retained, hierarchically pores-constructed and active materials-loaded for high-performance hybrid oxide supercapacitor

Min Luo,Kai Yang,Daotong Zhang,Chaozheng Liu,Pei Yang,Weimin Chen,Xiaoyan Zhou

Lignocellulose including cellulose , lignin, and hemicellulose could be extracted from wood, and has been used to prepare carbon electrode. However, complicated extraction greatly increases preparation cost. To achieve maximum utilization of lignocellulose and avoid complicated extraction, wood with porous structure and good mechanical strength is used as carbon precursor. Additionally, chemical activation is commonly used to create micropores to provide high capacitance, but it brings in natural structure destruction, and generation of wastewater during pickling. Moreover, to achieve desirable energy density, multi-step strategy with long duration is required for loading active materials on carbonized lignocellulose (CL). Herein, a one-step method is developed to prepare a free-standing hybrid CL electrode (CLE) by using Lewis acid in three aspects: (1) as structure protection agent, (2) as activating agent, (3) as active materials donor, which bypasses pickling and further avoids the generation of wastewater. Additionally, natural vessels in wood can not only provide large space for active materials loading, but also act as rapid ions diffusion way, simultaneously confining active materials detachment. Benefiting from the synergistic effect of porous structure and Lewis acid, this work not only makes full utilization of lignocellulose, but also makes CLE exhibit excellent performance in hybrid oxide supercapacitor.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Design of a porous lignocellulose-based hydrogel-Pd nanoparticles reactor system and its in-situ simultaneous adsorption-catalysis process concept for pollutant remedy

Lili Zhang,Hailong Lu,Jinxia Ma,Yimin Fan,Zhiguo Wang,Yonghao Ni

The separation and reusability of nano-catalysts are paramount for their high-efficiency and low-cost use. Herein, lignocellulose hydrogels (LCG), were fabricated and served as the host matrix for in-situ generated palladium nanoparticles (Pd NPs), creating hydrogel-based Pd NPs reactor systems. The lignocellulose hydrogel-based Pd NPs (LCG/Pd NPs) reactor system possesses the following unique features: (1) lignin present in LCG acts as a “green” reducing agent so that Pd NPs are formed in situ; (2) the in-situ generated Pd NPs are well dispersed in the LCG structure via complexation; (3) the simultaneous adsorption-catalysis process concept is very effective for pollutant remedy: the adsorption of pollutants on the porous LCG effectively increases the pollutant concentration on the reaction sites, where the Pd NPs are co-located, enhancing the catalytic reactions; as a result, a much higher catalytic reaction rate is observed; (4) the LCG/Pd NPs reactor systems are readily reused/recycled after each use. As proof of this concept, the catalytic performance of the LCG/Pd NPs reactor system was demonstrated by the catalytic reduction of toxic heavy metal ions (Cr 6+ ) and organic dye (methyl orange). Results showed that the novel LCG/Pd NPs reactor system exhibited much increased catalytic reduction rates: the pseudo-first-order rate constant (k) is 118 times higher (from 0.018 to 2.129 min −1 at 25 °C) for MO, and 38 times higher (from 0.008 to 0.304 min −1 at 25 °C) for Cr 6+ , in comparison with the control, under otherwise the same conditions.

CAS / MDL: 7529-22-8
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INDUSTRIAL CROPS AND PRODUCTS · 2024 · IF 5.6

Conversion of biomass to biofuels: Integration of a ternary deep eutectic solvent pretreatment and microbial fermentation for C2-C4 bioalcohols production from lignocellulose

Hongzhen Luo,Tairan Zhou,Rui Zhang,Qianyue Yang,Xinyan You,Shijie Wang,Jiabin Wang,Fang Xie,Rongling Yang

Efficient production of second-generation biofuels (bioethanol and biobutanol) from renewable lignocellulosic biomass holds strategic importance and aligns with sustainability objectives. However, it poses a persistent long-term challenge because of the biomass recalcitrance. Therefore, development of mild, environmentally friendly biomass pretreatment methods is a critical concern. To this end, in this study, a ternary deep eutectic solvent (DES) was synthesized with choline chloride , succinic acid , and glycerol at a molar ratio of 1:0.5:0.5. The ternary DES pretreatment largely enhanced glucan digestibility of corn stover (CS) to 94.7 % which was 4.60-fold to untreated CS. Mechanism of improved enzymatic efficiency of DES-pretreated CS was revealed by characterization methods such as SEM, XRD, and FTIR technologies. In addition, adding 1.0 % H 2 SO 4 to the ternary DES further increased enzymatic hydrolysis yield to nearly 100 %. Subsequently, the H 2 SO 4 -assisted DES-pretreated CS was used as substrate to produce C2-C4 bioalcohols (ethanol and butanol) by microbial fermentations. The results indicate that 46.6–49.2 g/L ethanol could be obtained by S. cerevisiae under separate hydrolysis and fermentation (SHF), and simultaneous saccharification and fermentation (SSF) strategies. Meanwhile, up to 11.9 g/L butanol was achieved from CS hydrolysate by Clostridium acetobutylicum with fed-batch mode. Finally, an artificial microbial consortium by co-culturing C. acetobutylicum and S. cerevisiae was developed which efficiently co-produced 12.4 g/L biobutanol and 5.7 g/L bioethanol from CS hydrolysate. Overall, this study provides a sustainable and green pretreatment technology that deconstruct lignocellulose and possess universality to produce various low-carbon bioalcohols by microbial fermentations.

CAS / MDL: 67-48-1
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MOLECULES · 2021 ·Vol. 26 ·期 13 ·3870 · IF 4.412

Diverse Banana Pseudostems and Rachis Are Distinctive for Edible Carbohydrates and Lignocellulose Saccharification towards High Bioethanol Production under Chemical and Liquid Hot Water Pretreatments

Jingyang Li,Fei Liu,Hua Yu,Yuqi Li,Shiguang Zhou,Yuanhang Ai,Xinyu Zhou,Youmei Wang,Lingqiang Wang,Liangcai Peng,Yanting Wang

Banana is a major fruit crop throughout the world with abundant lignocellulose in the pseudostem and rachis residues for biofuel production. In this study, we collected a total of 11 pseudostems and rachis samples that were originally derived from different genetic types and ecological locations of banana crops and then examined largely varied edible carbohydrates (soluble sugars, starch) and lignocellulose compositions. By performing chemical (H2SO4, NaOH) and liquid hot water (LHW) pretreatments, we also found a remarkable variation in biomass enzymatic saccharification and bioethanol production among all banana samples examined. Consequently, this study identified a desirable banana (Refen1, subgroup Pisang Awak) crop containing large amounts of edible carbohydrates and completely digestible lignocellulose, which could be combined to achieve the highest bioethanol yields of 31–38% (% dry matter), compared with previously reported ones in other bioenergy crops. Chemical analysis further indicated that the cellulose CrI and lignin G-monomer should be two major recalcitrant factors affecting biomass enzymatic saccharification in banana pseudostems and rachis. Therefore, this study not only examined rich edible carbohydrates for food in the banana pseudostems but also detected digestible lignocellulose for bioethanol production in rachis tissue, providing a strategy applicable for genetic breeding and biomass processing in banana crops.Keywords:banana;pseudostem;rachis;biomass pretreatments;enzymatic saccharification;bioethanol fermentation;cellulose crystallinity

CAS / MDL: 87-89-8 76-05-1
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Green Energy & Environment · 2024 · IF 10.7

Atmospheric reductive catalytic fractionation of lignocellulose integrated with one-pot catalytic conversion of carbohydrate yielding valuable lignin monomers and platform chemicals from corn straw

Meng-Ying Liu,Zhe-Hui Zhang,Xue-Qi Wang,Qian Sun,Chen Zhang,Yu Li,Zhuohua Sun,Katalin Barta,Feng Peng,Tong-Qi Yuan

Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years. Herein, taking advantage of the “lignin first” strategy, corn straw is converted to valuable chemicals including lignin monomers, furfural and 5-methoxymethylfurfural via a two steps process. The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol. The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives, thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up. In the initial step, depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%. Subsequently, in a dimethyl carbonate system, the carbohydrate component underwent complete conversion in a one-pot process, yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7 %.

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GREEN CHEMISTRY · 2023 ·Vol. 26 ·期 2 ·879-894 · IF 9.8

Weakening fibril–fibril interactions via an on-demand regulation of hemicellulose phase towards the facile disassembly of lignocellulose heterostructure into approaching native-state elementary fibrils

Yan Jiang,Xinyi Wang,Zhiqian Meng,Mengyang Zhang,Shuangfei Wang,Xiuyu Liu

It is of great technical interest but still challenging to develop a cost-effective and eco-friendly method to extract high-aspect-ratio elementary nanofibrils with native-state microstructure from recalcitrant lignocellulosic biomass because established chemical/biological/mechanical approaches inevitably give rise to the breakage of cellulose chains during the nanofibrillation of lignocellulose. Nature has designed hierarchical and heterogeneous lignocellulose structures, among which hemicellulose significantly affects interfibrillar interactions due to its unique molecular structure and micro-distribution pattern. Inspired by this fact, we amplify the hemicellulose stimulation effect on nanofibrillation using an on-demand regulated ionic liquid/water cosolvent and dissociate ultrahigh aspect ratio (2213) elementary fibrils (diameter = 4.7 nm) comprising approaching native-state structural carbohydrates from mildly delignified lignocellulose fibers (i.e. holocellulose) by a low-energy blender. We elucidated the mechanism for the exceptional disassembly behavior of holocellulose fibers: the high-level swelling of the amorphous and negatively charged hemicellulose phase weakens fibril–fibril interactions. The high-aspect-ratio morphology, well-preserved cellulose molecular structure, and hemicellulose-rich surface chemistry of the as-prepared nanofibrils significantly affect their self-assembly behavior and contribute to the extraordinary mechanical and optical performances of the corresponding nanopaper that conventional cellulose nano-papers/composites retain unsurpassed, e.g., overcome general conflicts between strength (310 MPa) and toughness (53 MJ m−3) and between transparency (86%) and haze (77%). This work provides a scale-up, ecologically and economically efficient lignocellulose nanostructure-engineered strategy for manufacturing high-performance structural nanomaterials towards a high-tech and carbon-neutral future.

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