INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Haoxiang Zhu,Youdi Zhang,Xusheng Guo,Youwei Cheng,Lijun Wang,Xi Li
5-Hydroxymethylfurfural (HMF) is a high-value biomass-derived platform chemical derived from renewable biomass, which is a great alternative to petroleum-based chemicals; however, it cannot be produced on a large scale at present because of the limitation of a low HMF yield and costly production. In this work, an experimental study of one-pot production of HMF from glucose in an acetone–water solvent was conducted. The effects of inorganic salts (in specific, NaCl) on miscible solvents were studied because inorganic salts could affect the phase structure of solvents. We also study the influence of the ratio between Lewis acid and Brønsted acid (L/B) on the dehydration reaction. After parameter optimization experiments, up to 64.5% HMF yield was obtained at the condition of C0 = 1.25 w/v %, CAlCl3 = 1.25 w/v %, CHCl = 10 mmol·L–1, T = 160 °C, and o/a = 80/20, and the optimized L/B was 1.25 kg·mol–1. Finally, an economic and efficient HMF production process including HMF purification and catalyst recycling was proposed; the HMF product could be produced and separated with high recovery (∼88%) and purity (∼85%) in the process. Our findings and analysis would provide support for the choice of the reaction system and bifunctional catalyst synthesis in the subsequent industrial demonstration development.
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Microbial Cell Factories
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2022
·Vol. 21
·期 1
·1-15
·
IF 6.352
Zhang Zhen,Yu Zichen,Wang Jinduo,Yu Yifa,Li Lanxiao,Sun Pengjie,Fan Xiaoguang,Xu Qingyang
Background 5-hydroxytryptophan (5-HTP), the direct biosynthetic precursor of the neurotransmitter 5-hydroxytryptamine, has been shown to have unique efficacy in the treatment of a variety of disorders, including depression, insomnia, and chronic headaches, and is one of the most commercially valuable amino acid derivatives. However, microbial fermentation for 5-HTP production continues to face many challenges, including low titer/yield and the presence of the intermediate L-tryptophan (L-Trp), owing to the complexity and low activity of heterologous expression in prokaryotes. Therefore, there is a need to construct an efficient microbial cell factory for 5-HTP production.Results We describe the systematic modular engineering of wild-type Escherichia coli for the efficient fermentation of 5-HTP from glucose. First, a xylose-induced T7 RNA polymerase-PT7 promoter system was constructed to ensure the efficient expression of each key heterologous pathway in E. coli. Next, a new tryptophan hydroxylase mutant was used to construct an efficient tryptophan hydroxylation module, and the cofactor tetrahydrobiopterin synthesis and regeneration pathway was expressed in combination. The L-Trp synthesis module was constructed by modifying the key metabolic nodes of tryptophan biosynthesis, and the heterologous synthesis of 5-HTP was achieved. Finally, the NAD(P)H regeneration module was constructed by the moderate expression of the heterologous GDHesi pathway, which successfully reduced the surplus of the intermediate L-Trp. The final engineered strain HTP11 was able to produce 8.58 g/L 5-HTP in a 5-L bioreactor with a yield of 0.095 g/g glucose and a maximum real-time productivity of 0.48 g/L/h, the highest values reported by microbial fermentation.Conclusion In this study, we demonstrate the successful design of a cell factory for high-level 5-HTP production, combined with simple processes that have potential for use in industrial applications in the future. Thus, this study provides a reference for the production of high-value amino acid derivatives using a systematic modular engineering strategy and a basis for an efficient engineered strain development of 5-HTP high-value derivatives.
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Catalysts
·
2022
·Vol. 12
·期 8
·901
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IF 4.501
Huaigang Su,Ze Zong,Wenjing Lou,Qin Zhao,Xiaobo Wang,Xiang Feng,Yanxing Qi,Zhaoning Song
In this study, Zr active species were implanted into a ZSM-5 zeolite framework to form a solid acid catalyst through steam treatment and the liquid-solid isomorphous substitution process. The as-synthesized Zr-ZSM-5-st catalyst ensured excellent esterification of trimethylolpropane and fatty acids (FAs) to achieve a polyol ester production yield of 94.41%. Combined with N2physisorption, X-ray diffraction, Fourier transform infrared spectroscopy, ultraviolet-visible spectroscopy, transmission electron microscopy mapping, X-ray photoelectron spectroscopy, NH3temperature-programmed desorption, and inductively coupled mass plasma spectroscopy were conducted. The results revealed that the excellent performance of Zr-ZSM-5-st catalyst could be attributed to the enhanced acidity and the developed surface area and pore structure.Keywords:Zr-containing solid acid catalyst;ZSM-5 zeolite;polyol ester;esterification;lubricating ester oils
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yuechao Yang,Danxia Xu,Baolong Zhang,Zhimin Xue,Tiancheng Mu
Electrochemical oxidation of alcohol and aldehyde to carboxylic acids is one of the most important classes of catalytic reaction. The key point for such reactions lies in the fine tailoring the catalysts to improve the reaction and energy efficiency. For such a destination, identifying descriptors which are highly related to the catalytic efficiency is a prerequisite for designing electrocatalysts. In this work, taking 5-hydroxymethylfurfural (HMF), a biomass derived platform molecule containing alcohol and aldehyde, as the main research object, we revealed for the first time that the adsorption energy of substrate molecule is an activity descriptor for electrochemical alcohol and aldehyde oxidation. Too weak substrate adsorption is not favorable to C–H/O–H bond activation and dissociation, while too strong substrate adsorption hinders the formation of enough OH ads (an important intermediate) due to the competitive adsorption of substrate molecules and OH – at limited reaction sites. The optimal catalytic activity can be achieved by adjusting the adsorption energy of substrate molecules to make them properly adsorbed on the catalyst surface. This work not only offers a guideline for the design of advanced catalysts towards the electrochemical alcohol and aldehyde oxidation (e.g., methanol, ethanol, benzyl alcohol, glycerol, glucose, furfural and HMF) for the utilization and production of renewable resources, but also benefits the design of other electrochemical catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Guoguang Wei,Yan Chen,Ning Zhou,Qiuhao Lu,Sheng Xu,Alei Zhang,Kequan Chen,Pingkai Ouyang
Enzyme cofactors are essential in biocatalysis for many enzymes. However, their high commercial cost limits the industrial application of cofactor-dependent enzymes. We overcame this challenge by constructing a self-sufficient biocatalyst that co-immobilised pyridoxal 5′-phosphate (PLP) and L-lysine decarboxylase (LDC) using natural polymer chitin as the functional material. First, degree of deacetylation (DDA) of chitin was regulated to enhance PLP adsorption and immobilisation. Then, the enzyme was immobilised via fusion of a chitin-binding domain. Chitin with 36% DDA efficiently co-immobilised LDC and PLP. Laser scanning confocal microscope and scanning electron microscope proved that the LDC and PLP were immobilised on the chitin. The self-sufficient biocatalyst retained over 55% of its original activity after five cycles. The proposed strategy provides a new way to achieve co-immobilisation of PLP-dependent enzymes.
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Molecular Catalysis
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2021
·
IF 5.062
Qian Wang,Jie Zhang,Wenlong Jia,Xin Yu,Jiahong Chen,Yong Sun,Zuojun Wei,Shuliang Yang,Xing Tang,Xianhai Zeng,Lu Lin
Generally, 5-hydroxymethylfurfural (HMF) is used as feedstock to produce 2,5-furandicarboxylic acid (FDCA). Whereas, its poor stability in alkaline environment results in low yield of FDCA. By contrast, 5-[(formyloxy)methyl]furfural (FMF), a novel platform compound derived from HMF, with higher thermal and alkaline stability than HMF, is more promising to replace HMF as substrate for the production of FDCA. In this study, FMF was successfully converted into FDCA over MoCuO x by using NaClO as oxidant, undergoing 2,5-diformylfuran (DFF) and 5-hydroxymethylfuran-2-carboxylic acid (HMFCA) as intermediates. Under optimization condition (30 min, 40 °C), 100% yield of FDCA was obtained. Furthermore, it was also demonstrated that the yield of FDCA up to 90% was gained in 5 wt % FMF concentration. Higher oxygen species mobility and lattice oxygen ratio endowed MoCuO x excellent catalytic activity. The synergy of Mo and Cu species in MoCuO x ensured an efficient conversion of HMF to FDCA through synergistic redox couple of Mo 6+ /Mo 5+ and Cu 2+ /Cu + .
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2021
·
IF 2.262
Xueshuai Chen,Rongli Jiang,Zihan Zhou,Xingwen Wang
In this work, ZSM-5 crystals with sheet-like morphology and well-dispersion were successfully synthesized from addition of green and cheap natural polymer (gelatin). The morphology and dispersion of crystals were related to the gelatin amount added to the synthesis gel, the three-dimensional pores of polymer hydrogels can serve as microreactors for controlling zeolite growth and dispersion in a confined space. Catalytic activity for the methanol to hydrocarbons (MTH) reaction of sample synthesized by adding gelatin at a gelatin/H2O mass ratio of 2% was better than that obtained from the synthesis gel free of gelatin. Its excellent catalytic performance can be attributed to the proper acidity, well-dispersion, and sheet-like morphology.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 18
·8306-8313
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IF 3.591
Hui Xu,Yue Xiao,Jinlu Tang,Dongfang Liu,Xinxin Shi,Aaron Albert Aryee,Hongmin Meng,Lingbo Qu,Zhaohui Li
Chemotherapy for cancer treatment is widely used but remains restricted by several limitations, including inefficient drug delivery and concomitant adverse side effects. Herein, we report a new prodrug-based self-assembled nanoparticle for the efficient treatment of cancer. Amphiphilic prodrug molecules (3′,5′-dioleoyl floxuridine, DOF) were constructed to form prodrug nanoparticles (DOF NPs) through a self-assembly process in water via hydrophobic interactions. The DOF NPs with high stability can be quickly enriched in tumor cells and release the floxuridine drug via hydrolysis of ester bonds by esterase. In vitro experiments reveal that the DOF NPs possess satisfactory tumor killing effects and weak toxicity and side effects. These unique features could further promote the research progress of prodrug-based self-assembled strategies for the application of chemotherapy in cancer.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Qian Wang,Huanshun Yin,Yunlei Zhou,Jun Wang,Shiyun Ai
As an important epigenetic modification, 5-formylcytosine (5fC) plays a vital role in cell differentiation, genomic DNA structure and function regulation. Its low abundance in all suckler tissues and cells and high structural similarity with cytosine (C) and its derivatives, the sensitive and selective detection method for 5fC is required. In this work, a photoelectrochemical biosensor was constructed using BiIO 4 -WS 2 composite as photosensitive material, the synergy of ternary heterojunction of BiIO 4 -WS 2 /CuO as signal amplification technology and 5-formylcytosine deoxyribonucleoside (5fdC) as target. Firstly, the ITO electrode modified by BiIO 4 -WS 2 was aminated by (3- aminopropyl) triethoxysilane. 5fC was captured on the electrode surface with amidogen as recognition reagent, based on the amide bond formed between amidogen and aldehyde group. Then, 4-carboxyphenylboronic acid (4-CPBA) was linked by covalent reaction between boronic acid and O -diol of 5fdC. Finally, the signal amplification material of amino-functionalized CuO was deposited on the electrode surface through the formation of amide bond based on −COOH of 4-CPBA and –NH 2 on CuO. In view of the constitution of a ternary heterojunction between CuO and BiIO 4 -WS 2 , the photoactivity of BiIO 4 -WS 2 was greatly enhanced, which also increased the detection sensitivity with the wide examination area from 0.005 to 200 nM and low limit of detection was 0.38pM (3σ). Based on the specific covalent identification pattern, this method showed high selectivity for 5fC, even discriminating 5fC with C and 5hmC. The impacts of antibiotics and heavy metals on 5fdC content change in genomic DNA of wheat tissues were investigated, and thus the feasibility of this work was evaluated.
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Journal of Environmental Chemical Engineering
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2021
·
IF 5.909
Junfei Liu,Hai Lin,Yingbo Dong,Yinhai He,Wei Liu,Yuanyuan Shi
The agglomeration and limited number of marginal adsorption sites have always been the restrictive factors for nano-MoS 2 adsorption performance. In this study, modified zeolite supported nano-MoS 2 (MoS 2 @Zeolite) with multiple adsorption sites was synthesized by combining ultrasonic and hydrothermal method, and utilized for tetracycline (TC) removal. MoS 2 @Zeolite-5 exhibits the best adsorption performance with a maximum saturation adsorption capacity of 396.70 mg g −1 (35 ℃). Meantime, MoS 2 @Zeolite-5 maintains a stable adsorption performance, which only decreased by 8.17% after four regeneration experiments. The structure characteristics and adsorption mechanism of adsorbents were also systematically investigated. The contact angle, crystal structure, micro-morphology analyses prove that modified zeolite plays the roles of enhancing the hydrophilia, restricting the growth of MoS 2 along C-axis, and exposing more adsorptive sites of MoS 2 . The Pseudo-second order kinetics is suitable for the model adsorption process and the adsorption process is endothermic. The adsorption mechanism of composites mainly relied on the chelation by Mo and electrostatic interaction. Furthermore, the effect of H-bonding and π-π action also existed. This study confirms that MoS 2 @Zeolite-5 is an efficient, stable, and promising adsorbent to treat TC-pollution of pharmaceutical wastewater.
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ANALYTICAL CHEMISTRY
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2021
·
IF 6.986
Jinmin Wang,Xianglong Qu,Limin Zhao,Bing Yan
Covalent organic framework (COF) nanosheets (NSs) are a new member in the family of two-dimensional (2D) nanomaterials that received increasing attention. The ability to prepare COF NSs with rapid acquisition is of great importance to explore their distinctive properties and potential applications. Herein, we elaborate design a new COF hybrid material EB-TFP:Eu(BTA)4 as a sensing platform. In the process of ratiometric fluorescence detection of 5-fluorouracil (5FU), an anticancer drug, we realize the preparation of COF NSs. Interaction occurs between 5FU and COF hybrid material, where the interlayer π–π stacking of COF was weakened, benefiting the exfoliation of bulk COF to acquire 2D COF NSs. This strategy provides not only a sensitive and selective 5FU sensor but also a significant inspiration for engineering 2D COF NSs.
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 7
·1984-1992
·
IF 2.482
Wu Ningxin,Zhang Manling,Pan Xiaomei,Zhang Jin,Gao Lijing,Xiao Guomin
Abstract The production of 5-hydroxymethylfurfural (HMF) from cellulose is of great significance for the high-value utilization of biomass, although this route currently faces the challenge of low efficiency. In the present work, a series of effective (x)Hf/ZSM-5 catalysts were developed for HMF production from cellulose, and analyzed by BET, XRD, SEM, ICP, NH 3 -TPD, Py-FTIR techniques. Driven by the (5)Hf/ZSM-5 catalyst, HMF with a yield of up to 67.5% and 17.2% of furfural are simultaneously obtained from cellulose in the H 2 O (NaCl) /THF biphasic system. Moreover, after four consecutive cycles, (5)Hf/ZSM-5 catalyst still maintained part of its catalytic activity. The 67.5% HMF yield achieved herein is one of the highest yields achieved in the conversion reaction using cellulose as a substrate, and the catalytic performance of the H 2 O (NaCl) /THF system containing the (5)Hf/ZSM-5 catalyst is even comparable to that of the expensive ionic liquid system. This result reflects the application prospect of (5)Hf/ZSM-5 catalyst in the future industrial production process of HMF. Graphic Abstract
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危险品化学品经营许可证（带存储）