APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 107
·期 5
·1751-1764
·
IF 5
Hamouda Hamed I.,Fan Yi-Xuan,Abdalla Mohnad,Su Hang,Lu Ming,Li Fu-Li
Abstract Lam16A is a novel GH16 β-1,3–1,4-lichenase isolated from the genus Caldicellulosiruptor which can utilize untreated carbohydrate components of plant cell walls. Its catalytic module has been characterized that the six carbohydrate-binding modules (CBMs) were queued in the C-terminus, but their roles were still unclear. Here, full-length and CBM-truncated mutants of Lam16A were purified and characterized through heterologous expression in Escherichia coli . The profiles of these proteins, including the enzyme activity, degrading efficiency, substrate-binding affinity, and thermostability, were explored. Full-length Lam16A with six CBMs showed excellent thermostability and the highest activity against barley β-glucan and laminarin with optimum pH of 6.5. The CBMs stimulated degrading ability of the catalytic module, especially against β-1,3(4)-glucan-based polysaccharides. The released products from β-1,3–1,4-glucan by Lam16A or its truncated mutants revealed an endo-type glycoside hydrolase. Lam16As exhibited strong binding affinities to the insoluble polysaccharides, especially Lam16A-1CBM. The degradation of yeast cell walls by Lam16A enzyme solution relative to the control reduced the absorbance values at OD 800 by ~ 85% ± 1.2, enabling the release of up to ~ 0.057 ± 0.0039 µg/mL of the cytoplasmic protein into the supernatant, lowering the viability of the cells by ~ 70.3% ± 6.9, thus causing significant damage in the cell wall structure. Taken together, CBMs could influence the substrate specificity, thermal stability, and binding affinity of β-1,3–1,4-glucanase. These results demonstrate the great potential of these enzymes to promote the bioavailability of β-1,3-glucan oligosaccharides for health benefits.
Key points
Carbohydrate-binding modules strongly influenced the enzyme activity and binding affinity, and further impacted glycoside hydrolase activity.
Lam16A enzymes have sufficient ability to hydrolyze β-1,3–1,4-glucan-based polysaccharides.
Lam16As provide a powerful tool to promote the bioavailability of β-1,3-glucan oligosaccharides.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Qiang Lu,Yuefang Chen,Weipeng Song,Chaonan Tao,Junhua Zhang,Yong Sun,Lincai Peng,Huai Liu
Direct utilization of cellulosic material to produce specialty chemicals such as levulinate ester could greatly increase biorefinery profitability, but low-level efficiency due to its structural nature limits the strategy for industrial deployment. We report herein that adding γ-valerolactone (GVL) co-solvent during the acid-catalyzed conversion of cellulose in ethanol leads to a high reaction rate and improved catalytic activity towards ethyl levulinate (EL) production. With GVL as the co-solvent (the volume ratio of GVL to ethanol in 1:4), the yield of EL highly enhanced from 31% to 56% under mild operating conditions (170 °C for 2 h) over a low loading Al(OTf) 3 of 0.005 mol/L. The mechanistic role of GVL co-solvent to accelerate EL formation from cellulose has been fully elucidated via the combination of experimental and theoretical approaches. It demonstrates that GVL intervention not only favored the dissolution and depolymerization of cellulose, but also enabled the formation of Al species with higher acidity and catalytic activity by modulating the solvation environment, both of which are in charge of promoting cellulose conversion to EL. The activation energy barriers for cellulose depolymerization and glucoside alcoholysis have decreased by 30.8 kJ/mol and 24.8 kJ/mol, respectively. The understanding of this solvation effect can be employed to optimize the rate and yield for production of the versatile bio-based ester compound straight from cellulose valorization.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Binbin Zhang,Jiao Ma,Kaide Ou,Xin Cong,Hao Zou,Yonggui Liao,Yajiang Yang,Hong Wang
By loading 3-nitrophenylboronic acid (3-NPBA) which can react with saccharide, the fluorescence lanthanide metallogel can emit fluorescence signals at 398, 490 and 546 nm. Thus, a three-dimensional responsive fluorescence sensor array (H 6 L/Tb 3+ /3-NPBA) was prepared to recognize saccharides. Due to the typical pH responsiveness of the fluorescence behavior of the sensor array, it is suitable for H + generation systems, such as the reaction of 3-NPBA with cis -diol of saccharides. The response of fluorescence signal intensity to 15 different saccharides was measured, and the qualitative discrimination of those saccharides was investigated by principal component analysis (PCA). The results showed that PCA elliptic clusters did not overlap, even though the concentration of the saccharides was as low as 3 mmol/L, and the discrimination rate of each saccharide reached 100 %. The “double blind” experiment indicated that the sensor system has good ability to discriminate unknown component samples. Furthermore, the discrimination rate of fructose/glucose mixtures with varied mole ratios also reached 100 %. The method of Euclidean distance confirmed that there was a good linear correlation between PCA elliptic clusters of fructose and its concentration, which could realize the quantitative analysis of fructose. The results of PCA indicated that the elliptic clusters of tea drinks with various sugars and commercially available sugar-containing drinks were loosely distributed, which further confirmed that the sensor system can effectively discriminate the saccharides under the interference of complex components.
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2023
·
IF 10.9
Yuewen Dai,Maofu Geng,Yuhong Tao,Zhenyu Zhang,Chengqi Feng,Juncheng Huang,Fei Liu,Haining Na,Jin Zhu
By catalytically converting cellulose using a phosphate-modified hydroxyl-rich carbon-based catalyst (P@HRCBC), which was made by hydrothermal carbonization , glucose was successfully hydrolyzed from cellulose in an aqueous phase system (HTC). The glycosidic bond breaking catalyzed by the -PO 3 H 2 and the cellulose matrix lamellar exfoliation are both enhanced by the excellent adsorption capacity of the exceptionally rich –OH. The activity of cellulase is perfectly imitated. Within 120 min, the glucose output and the conversion of cellulose achieved 96.3% and 47.1%, respectively. The numerous ways that P@HRCBC adsorbs cellulose and cellobiose alter its catalytic ability and make separating glucose easier. After numerous cycles, the conversion of cellulose was maintained at 90.3%, thanks to the remarkable stability of –OH and -PO 3 H 2 . P@HRCBC shows an actual "enzymatic" catalytic function that provides a new solution for the efficient green hydrolysis of cellulose into glucose.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Jingwen Wang,Xiaoshuai Han,Weijie Wu,Xiaoyi Wang,Linhu Ding,Yuli Wang,Shanshan Li,Jiapeng Hu,Weisen Yang,Chunmei Zhang,Shaohua Jiang
Wooden building materials have advantages in terms of biodegradability , non-toxicity, pollution-free and recycling. Currently, applications of natural wood are extremely limited because of low density, low strength and toughness. Therefore, we reported an effective modification strategy with nano-scale cellulose nanofibrils design to prepare a synergistically enhanced cellulosic material . Via three steps: i) the secondary alcohol hydroxyl groups in C 2 , C 3 position were cut; ii) oxidize the hydroxyl group at C 2 , C 3 position to achieve dialdehyde cellulose; and iii) oxidized again to obtain dicarboxylic cellulose. Subsequently, thanks to the regulation of the average moisture content, the moisture content in the wood surface and subsurface increased in a short time. The wood softening layer contributes to the hotpressing treatment of the wood. The mechanical properties and dimensionality have been greatly improved. The obtained delignified oxidated hot-pressed wood with 0.55 mmol/g carboxyl group content demonstrates excellent strength of 328.8 ± 7.43 MPa and Young's modulus of 8.1 ± 0.14 GPa, which is twice than that of natural wood. Delignified oxidated hot-pressed wood also shows exceptional toughness of 8.3 ± 0.28 MJ/m 3 . Other than that, the shore hardness indicates 0.55 mmol/g carboxylic group, which could increase the hardness at the wood surface hardness to 72.5 ± 4.29°.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIOMASS & BIOENERGY
·
2023
·
IF 6
Jirui Yang,Yanwei Zhang,Feng Shen,Xinhua Qi
Meerwein-Ponndorf-Verley (MPV) reaction has been widely acknowledged to be a mild catalytic transfer hydrogenation method for selective reduction of biomass-derived furfural to furfuryl alcohol . Herein zirconium-containing mesoporous composite catalyst was developed through the combination of sol-gel process and soft templating method, in which naturally abundant glucose and F127 triblock copolymer were used as the ligand and pore-forming agent, respectively. The hydroxyl groups in glucose molecules were demonstrated to be coordinated with zirconium ion during hydrolysis-condensation of zirconium precursor, leading to the even dispersion of zirconia nanoparticles in the composite catalyst. The composite catalyst was proven to be highly efficient for catalyzing MPV reduction of furfural with the maximum furfuryl alcohol yield of 93.4% at 180 °C within 180 min in 2-propanol, which served as both solvent and reductant . The composite also showed a good reusability . After five consecutive reaction cycles, furfuryl alcohol yield was slightly reduced from 93.4% to 77.7%, but it could be recovered to 92.8% after the reused composite was regenerated with dilute alkali solution. Batch experiments and systematic characterizations demonstrated that the excellent catalytic performance of composite catalyst was determined by multiple factors mainly including the stronger Lewis acidity, a considerable amount of basic site and the rich mesoporous structure. This study provides a facile strategy to prepare multifunctional composite catalysts using naturally abundant carbohydrates as the feedstocks for lignocellulosic biorefinery .
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Rui Jiao,Yanming Wang,Yuxia Pang,Dongjie Yang,Zhixian Li,Hongming Lou,Xueqing Qiu
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 (Fe2+) 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 (Fe2+–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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Rongfan Ren,Minghui Yuan,Hongli Li,David Da Yong Chen
Carbohydrates play critically important roles in energy supply and biological functions in living systems. However, it has been a great challenge to identify saccharides and distinguish their isomers because they have highly similar structures and many possible positions for glycosidic linkages. In this work, an ambient ionization tandem mass spectrometry method was developed to characterize disaccharide structural isomers with in situ methylation. The direct analysis in real time ion source can be used to facilitate the methylation reaction of disaccharides with tetramethylammonium hydroxide. The hydroxyl groups of disaccharides can be methylated instantaneously, and the products can be ionized at the same time. The methylated product ions from full scan mass spectrometry (MS) and tandem MS can be used to distinguish a variety of disaccharide structural isomers with different glycosidic linkages, compositions, and configurations. Characteristic marker ions were discovered, and they can be used for the assignment of linkage type and identification of specific isomeric forms. The method was used for the direct identification of disaccharide isomers from real commercial products such as honey, wine, and milk without complex sample pretreatment or chromatographic separation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Hong Liu,Chengqi Feng,Zewei Gong,Yuxin Zhu,Juncheng Huang,Yafei Li,Haining Na,Jin Zhu
Raspberry-like carbon layer coated silica nanoparticles (MSN-x-NH 2 @C) with controllable hydroxyl-rich rough surface is designed and synthesized by use of alkaline etching strategy and hydrothermal carbonization (HTC) method, which is utilized as catalyst to provide particular interaction with cellulose between the solid-solid interfaces. Through the control of surface roughness of the raspberry-like catalyst, it induces the formation of local area with strong absorption on the surface and thus enhance the capability to disrupt the aggregated structure of cellulose. Accordingly, in low acidic aqueous system with MSN-x-NH 2 @C, the cellulose conversion rate is up to 91.99% with the total reducing sugar yield at 81.46% and glucose yield of ∼70% after the second hydrolysis in aqueous system. Furthermore, the obtained MSN-x-NH 2 @C exhibits good thermal stability and reusability. This research provides a new perspective for the design and preparation of nano-sized solid catalyst with controlled surface topological structure to enable the surface adsorption capability towards cellulose more efficiently in aqueous system.
✓ 已验证
产品关联
DOI
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2023
·
IF 3.4
Shuaifeng Liu,Meng Zhang,Dengwang Hong,Zemin Fang,Yazhong Xiao,Wei Fang,Xuecheng Zhang
β-Glucosidases with high catalytic activity and glucose tolerant properties possess promising applications in lignocellulose-based industries. To obtain enzymes possessing these properties, a semi-rational strategy was employed to engineer the glucose-stimulating β-glucosidase Bgl2A for high cellobiose hydrolysis activity. A total of 18 mutants were constructed. A22S, V224D, and A22S/V224D exhibited high specific activities of 272.06, 237.60, and 239.29 U/mg toward cellobiose, which were 2.5- to 2.8-fold of Bgl2A. A22S, V224D, and A22S/V224D exhibited increased k cat values, which were 2.7- to 3.1-fold of Bgl2A. A22S and V224D maintained glucose-stimulating property, whereas A22S/V224D lost it. Using 150 g/L cellobiose as the substrate, the amount of glucose produced by A22S was the highest, yielding 129.70 g/L glucose after 3 h reaction at 35 °C. The synergistic effects of the engineered enzymes with commercial cellulase on hydrolyzing cellulose were investigated. Supplemented with the commercial cellulase and A22S, the highest glucose amount of 23.30 g/L was yielded from cellulose with hydrolysis rate of 21.02 %. Given its high cellobiose hydrolysis activity and glucose-stimulating properties, A22S can be used as a component of enzyme cocktail to match mesophilic cellulases for efficient cellulose hydrolysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
·
2023
·Vol. 37
·期 18
·e9603
·
IF 2
Weiyang Zhang,Jing Cai,Wenqing Gao,Renlu Han,Haixing Wang,Yanfei Wu,Jiawei Wu,Yong Wu,Chenlu Wang,Keqi Tang,Jiancheng Yu
Rationale In the field of separation science, ion mobility spectrometry (IMS) plays an important role as an analytical tool. However, the lack of sufficient structural resolution is a common problem in qualitative and quantitative analysis using IMS. A method is needed to solve the problem of overlapping peaks caused by insufficient resolution. Methods The method uses multiple strategies to more effectively use population information to balance exploration and exploitation capabilities, prevent local optimization, accurately resolve overlapping peaks, quickly obtain optimal spectral peak model coefficients, and accurately identify compounds. Results Multistrategy JAYA algorithm's (MSJAYA) performance is compared with improved particle swarm optimization (IPSO), dynamic inertia weight particle swarm optimization (DIWPSO), and multiobjective dynamic teaching-learning-based optimization (MDTLBO). The analysis shows that MSJAYA's maximum separation error is within 0.6%, a level of accuracy not guaranteed by the other algorithms. In addition, the separation error fluctuates within a much smaller range, demonstrating MSJAYA's superior robustness. Conclusions Compared with other overlapping peak separation algorithms, MSJAYA is more applicable because no special parameters are used. The method allows fast deconvolution analysis of strong overlapping peaks with multiple components, which greatly improves the resolution of IMS.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Chihe Sun,Wenbo Wu,Haixing Chang,Rupeng Wang,Ke Wang,Nianbing Zhong,Ting Zhang,Xuefeng He,Fubao Sun,Ezhen Zhang,Shih-Hsin Ho
This study proposed a mild chlorination-sulfonation approach to synthesize magnetic carbon acid bearing with catalytic SO 3 H and adsorption Cl bifunctional sites on polydopamine coating. The catalysts exerted good textural structure and surface chemical properties (i.e., porosity, high specific surface area of >70 m 2 /g, high catalytic activity with 0.86–1.1 mmol/g of SO 3 H sites and 0.8%–1.9% of Cl sites, and abundant hydrophilic functional groups), rendering a maximum cellobiose adsorption efficiency of ∼40% within 6 h. Moreover, the catalysts had strong fracture characteristics on different α–/β–glycosidic bonds with 85.4%–93.9% of disaccharide conversion, while selectively fractionating hemicellulose from wheat straw with 64.3% of xylose yield and 93.4% of cellulose retention. Due to the stable interaction between parent polydopamine support with Fe core and functional groups, the catalysts efficiently recovered by simple magnetic separation had good reusability with minimal losses in catalytic activity.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）