CARBOHYDRATE POLYMERS
·
2019
·
IF 6.044
Chunfu Shao,Qiang Shao,Xiaoyi Wang,Jun Ling,Xiao Guo,Yulin Ning,Yujie Dai,Shiru Jia,Yuanyuan Qiao,Changwen Li,Kai Zhao
The OH induced cellulose degradation was examined by analyzing the reaction products of Fenton’s regents with cellobiose. Many degradation products including C2-C5 compounds such as oxaldehyde, malonaldehyde and 2-hydroxysuccinaldehyde were detected by GC MS analysis. Four reaction pathways for the formation of some degradation products were obtained from ReaxFF kinetics simulation and validated by the DFT quantum chemistry calculation at B3LYP/6-31+g(d,p) level. It was found that the H-abstraction from OH of the glucose unit by OH can cause saccharide ring open and breakage of the glycosidic bond. Pathways 1–4 showed that the glucose unit can react with OH consecutively to produce small molecular products with carbon atoms less than 6. This study indicated that ReaxFF reaction kinetics is a powerful tool for the exploration of the degradation mechanism of cellulose induced by OH at room temperature, which correlated well with the experimental results and was validated by DFT calculation.
研究领域:
生物化学
·
计算化学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS COMMUNICATIONS
·
2012
·
IF 2.986
Jun Zhang,Shubin Wu,Bo Li,Hongdan Zhang
Ru/C catalyst and extremely low phosphoric acid were used for direct conversion of cellobiose into sorbitol under hydrogen atmosphere. Effects of various parameters and catalyst reuse on the reaction performance were investigated in detail. An optimized sorbitol yield of 87.1% was attained at 458 K and 3 MPa H 2 for 1 h with catalyst usage of 15% in 0.05 wt.% phosphoric acid. The physicochemical properties of used Ru/C catalysts were characterized with various techniques to explore the specific causes for deactivation.
研究领域:
催化化学
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生物质转化
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应用化学
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能源化学
·
绿色化学
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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.
研究领域:
生物化学
·
酶工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Qidong Hou,Yifan Nie,Xiaoran Zhang,Ruite Lai,Xinyu Bai,Chao Xie,Hengli Qian,Guanjie Yu,Tianliang Xia,Yao Tang,Chengxu Wang,Fei Qu,Haixin Guo,Meiting Ju
The conversion of biomass-derived carbohydrates to 5-ethoxymethylfurfural (EMF) is a fascinating reaction with 100% carbon atom utilization. Although effective conversion of 5-hydroxymethylfurfural (HMF) and fructose to EMF have been achieved, the direct conversion of glucose only gave low EMF yields. Herein, we reveal that the combinations of common Lewis acid with Brønsted acid in ethanol universally catalyze rapid etherification of glucose to intractable ethyl glucoside (EGL), as impedes the further conversion toward the desired products. The synergy of large-pore tin phosphate (SnPO) bearing strong Lewis acidic sites with acidic ionic liquid 1-(4-sulfobutyl)-3-methylimidazolium chloride (BSO 3 HMIMCl) enable tandem catalytic conversion of glucose, cellobiose and starch to EMF with record yields (61.7%, 61.8% and 55.7%, respectively), far exceeding previous reports. This transformation probably occurs via multiple parallel pathways, where water molecules generated by dehydration cooperate with acid and Cl - to hydrolyze EGL back to glucose, thus forming a positive feedback on EMF production.
研究领域:
化学工程
·
催化科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2016
·
IF 4.012
Hua Wang,Yingge Guo,Cuirong Chang,Xinli Zhu,Xiao Liu,Jinyu Han,Qingfeng Ge
The number of strong acid sites on a hydrolysis catalyst accessible by the bulky cellulose limits its efficiency in the conversion and utilization of biomass-based resources. In this work, high surface area WZr/SBA-15 catalysts (>400 m 2 /g) were prepared by hydrothermal method and characterized using XRD, N 2 adsorption, TEM, Raman, UV–vis, XPS and FTIR of pyridine adsorption. The results showed that doping a moderate amount of ZrO 2 into the WO 3 /SBA-15 catalyst stabilized the tungstate species in the form of a polytungstate species as a result of the strong ZrO x -WO x interaction as well as increased the surface area of the catalyst. The resulting polytungstate species provided strong Brønsted acid sites for hydrolysis. Consequently, the cellobiose conversion was maximized at 5% ZrO 2 loading, corresponding to a maximized surface area and density of Brønsted acid sites. This catalytic activity is significantly higher than that of a WO 3 /ZrO 2 catalyst prepared using the conventional impregnation method, indicating the importance of mesoporous structure to the dispersion of active species and to the accessibility of the active sites by the bulky reactant. This result indicates that the density of the strong Brønsted acid sites with improved accessibility by the bulky reactant is essential to achieve a high hydrolysis activity.
研究领域:
化学工程
·
催化材料
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产品关联
DOI
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2024
·
IF 3.4
Bohua Wang,Song Lei,Qingqin Li,Yushuang Luo
Lactulose is a semisynthetic nondigestive sugar derived from lactose, with wide applications in the food and pharmaceutical industries. Its biological production routes which use cellobiose 2-epimerase (C2E) as the key enzyme have attracted widespread attention. In this study, a set of C2Es from different sources were overexpressed in Escherichia coli to produce lactulose. We obtained a novel and highly efficient C2E from Clostridium disporicum (CDC2E) to synthesize lactulose from lactose. The effects of different heat treatment conditions, reaction pH, reaction temperature, and substrate concentrations were investigated. Under the optimum biotransformation conditions, the final concentration of lactulose was up to 1.45 M (496.3 g/L), with a lactose conversion rate of 72.5 %. This study provides a novel C2E for the biosynthesis of lactulose from low-cost lactose.
研究领域:
生物技术
·
食品科学
·
药学
·
酶学
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DOI
PubMed
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2025
·
IF 3.7
Haotian Cheng,Yuan Li,Yi Zhou,Shuke Wu,Yi-Heng P. Job Zhang
Cellobiose phosphorylase (CBP) catalyzes the reversible phosphorolysis of cellobiose to glucose and α-D-glucose-1-phosphate. CBPs play an important role in the in vivo enzymatic utilization of cellulosic materials. Here we discovered a novel CBP from Thermoclostridium caenicola (TcCBP), displaying 50–75 % sequence homology with previously reported CBPs. Recombinant TcCBP was well expressed in E. coli BL21(DE3), with a 1.6-fold increase in soluble expression levels over the widely-used Clostridium thermocellum CBP (CtCBP). This enzyme exhibited broad pH adaptability, maintaining substantial activities across pH 4.0–7.5 in the synthetic direction and pH 5.0–7.5 in the phosphorolytic direction. Compared to CtCBP, TcCBP displayed the superior thermostability and a nearly 100-fold improvement in "Product-to-Enzyme Ratio" (PE value). The biosynthesis of myo -inositol from cellobiose was conducted by using this CBP along with other four thermophilic enzymes (i.e., phosphoglucomutase, inositol 1-phosphate synthase, inositol monophosphatase, and polyphosphate glucokinase) in one pot without step-by-step addition of enzymes. Approximately 96 mM of myo -inositol was produced from 50 mM of cellobiose. These results indicated that this enzyme could be a potential thermophilic enzyme used for the production of value-added biochemicals by in vitro BioTransformation.
研究领域:
酶工程
·
分子生物学
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合成生物学
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代谢工程
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工业生物技术
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DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Fulong Zhang,Xu Zeng,Wu Lan,Xuejin Zhang,Chuanfu Liu
The enzymatic hydrolysis of pretreated lignocellulose to produce value-added oligosaccharides presents the advantages of a simplified procedural approach with reduced environmental impact. The subsequent purification is necessary to improve the purity of oligosaccharides for further application. In this work, a high-yield xylooligosaccharides-rich hydrolysate was obtained by ball-mill-assisted alkaline peroxide (BAP) pretreatment and enzymatic hydrolysis, and the sequential separation of xylobiose and cellobiose was performed by activated carbon adsorption. Adsorption kinetics and isotherm models of saccharides on activated carbon were systematically investigated to understand the adsorption behavior. Results indicate that separation achieves a purity exceeding 70 %, with 38.21 % of xylobiose and 84.22 % of cellobiose being adsorbed. Density functional theory (DFT) calculations reveal the involvement of oxygen-containing groups on the activated carbon surface in sugar adsorption from the molecular level. The findings of this study establish a theoretical foundation for separating xylobiose and cellobiose from oligosaccharides hydrolysate through activated carbon adsorption.
研究领域:
生物化学
·
可再生资源工程
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产品关联
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·
IF 6.7
Hao Fang,Yuan Li,Haotian Cheng,Shiyi Song,Fuping Lu,Yi-Heng P. Job Zhang
Lacto-N-biose I (LNB), a core structural unit of human milk oligosaccharides, was usually fermented by microbial cell factories because its biosynthesis involved the supplies of ATP and UDP-sugars. Here we designed an in vitro ATP- and UDP-sugar-free enzymatic pathway for the biosynthesis of LNB from lactose and N-acetylglucosamine (GlcNAc). Thermoclostridium caenicola cellobiose phosphorylase was discovered to have a very high promiscuous activity of lactose phosphorylase. Its lactose phosphorylase activity was enhanced greatly by directed evolution, yielding the variant M2 (N654A/Y501A) having 1.56-fold higher lactose activity and doubled lactose/cellobiose specificity. The coenzyme-free three-enzyme molecular machine containing lactose phosphorylase M2, lacto-N-biose phosphorylase and polyphosphate glucokinase produced up to 115 g/L LNB from lactose and GlcNAc and exhibited the highest volumetric productivity of 14.4 g/L/h. This coenzyme-free multienzyme molecular machine could provide a cost-competitive platform for in vitro biomanufacturing of LNB.
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DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL MICROBIOLOGY & BIOTECHNOLOGY
·
2022
·Vol. 49
·期 3
·
IF 4.258
Wang Lei,Zheng Peng,Hu Meirong,Tao Yong
Cellobiose, a natural disaccharide, attracts extensive attention as a potential functional food/feed additive. In this study, we present an inorganic phosphate (Pi) self-sufficient biotransformation system to produce cellobiose by co-expressing sucrose phosphorylase (SP) and cellobiose phosphorylase (CBP). The Bifidobacterium adolescentis SP (BASP) and Cellvibrio gilvus CBP (CGCBP) were co-expressed in Escherichia coli. Escherichia coli cells containing BASP and CGCBP were used as whole-cell catalysts to convert sucrose and glucose to cellobiose. The effects of reaction pH, temperature, Pi concentration, and substrate concentration were investigated. In the optimum biotransformation conditions, 800 mM cellobiose was produced from 1.0 M sucrose, 1.0 M glucose, and 50 mM Pi, within 12 hr. The by-product fructose and residual substrate (sucrose and glucose) were efficiently removed by treatment with yeast, to help purify the product cellobiose. The wider applicability of this Pi self-sufficiency strategy was demonstrated in the production of laminaribiose by co-expressing SP and laminaribiose phosphorylase. This study suggests that the Pi self-sufficiency strategy through co-expressing two phosphorylases has the advantage of great flexibility for enhanced production of cellobiose (or laminaribiose).
研究领域:
生物技术
·
生物化学
·
微生物学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 110
·90904-90912
·
IF 3.84
Yueling Cao,Junwei Wang,Maoqing Kang,Yulei Zhu
Hydrogenolysis of glucose and cellobiose, used as the model feedstocks, over Ni–WO3/SBA-15 catalysts has been investigated to probe the influencing factors for the conversion of cellulose to ethylene glycol (EG). The conversion of glucose and cellobiose to EG showed different dependencies on reaction temperature; a lower reaction temperature was needed for the former. Additionally, the surface atomic ratio of W to Ni on the Ni–WO3/SBA-15 catalysts was the key factor for the product distribution. Both glucose and cellobiose had their own optimum W–Ni ratio for the production of EG, and the ratio of W to Ni for glucose was slightly lower than that of cellobiose. On the other hand, the Ni–WO3/SBA-15 catalysts were thoroughly characterized by N2 adsorption–desorption, X-ray diffraction (XRD), hydrogen-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The results indicated that the reducibility of Ni–WO3/SBA-15 catalysts with high Ni loading was more similar to that of pure NiO. More importantly, the change of surface atomic content of Ni and W of Ni–WO3 catalysts with various Ni loadings resulted from the surface W species of the catalysts being gradually covered by Ni species with the increase of Ni loading.
研究领域:
化学工程
·
催化转化
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Niuniu Zhu,Manyu Zhang,Guo Qiu,Hongyu Tian,Yongguo Liu
The synthesis of platform chemical 5-hydroxymethylfurfural (5-HMF) provides favorable and efficient paths for the utilization of renewable biomass resources. In this work, highly active niobium-modified montmorillonite (Nb-Mont) catalysts were synthesized by a facile and ion-exchange method and were used for the one-pot conversion of cellobiose and sucrose to 5-HMF with optimal results. 5-HMF yield of 68.6% was obtained from cellobiose in a methyl isobutyl ketone (MIBK)/saturated salt water (SSW) biphasic solvent at 170 °C after 3 h. With sucrose as substrate in DMSO at 140 °C after 2 h, 5-HMF yield was 65.4%. The presence of Lewis and Brønsted acid sites on Nb-Mont facilitate the hydrolysis of cellobiose and sucrose and play essential roles in the subsequent isomerization of glucose monomer and the dehydration of fructose monomer. A possible reaction mechanism was proposed for the transformation of cellobiose and sucrose into 5-HMF, and the isomerization process of glucose monomer was the most critical step, confirmed by density functional theory (DFT) calculations. [NbO(OH) 2 ] + species as active sites could effectively reduce the activation energy of the isomerization process, which accelerated the synergetic proton transfer process. Nb-Mont was recycled at least four times without a prominent loss in the catalytic activity. In this study, a promising catalytic strategy was provided for heterogeneous Nb containing catalysts used in the effective synthesis of 5-HMF from carbohydrates.
研究领域:
化学工程
·
催化
·
可再生能源
·
材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）