GREEN CHEMISTRY
·
2022
·Vol. 24
·期 22
·8691-8704
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IF 11.034
Xin Pan,Xue Wang,Sihua Wu,Lei Xu,Leilei Zhang,Zhan Zhang,Bingfeng Li,Xuejun He,Siyuan Chang
Upgrading of the bio-based platform chemical 5-hydroxymethylfurfural (HMF) into high-value derivatives is an important research topic, particularly in green and sustainable chemistry. Herein, we applied a new, highly HMF-tolerant strain, Enterobacter ludwigii YYP3, as a whole-cell biocatalyst for efficient reduction of HMF to 2,5-bis(hydroxymethyl)furan (BHMF). Upon process optimization, within only 3 h, BHMF was produced with a yield >99% and 98.5% selectivity using 100 mM HMF, resulting in the highest space time yield (4.2 g L−1 h−1) among the currently reported HMF bioreduction processes. In a fed-batch conversion, E. ludwigii YYP3 achieved large-scale production of 290 mM BHMF within 9 h and retained its high catalytic activity for three runs (27 h), suggesting an excellent cycling stability. Based on genome and transcriptome analysis, the molecular mechanism underlying the high HMF tolerance of E. ludwigii YYP3 was explored, primarily through the downregulation of genes related to amino acid biosynthetic and metabolic processes and upregulation of genes associated with DNA replication, recombination, and repair; biofilm formation; and redox homeostasis. Meanwhile, two novel short-chain dehydrogenase/reductase family oxidoreductases ElSDR-ykvO and ElSDR-SSP1627 were identified as target enzymes responsible for conversion of HMF to less toxic BHMF in E. ludwigii YYP3. Combined with structure and mutation analysis, the catalytic mechanisms of target enzymes were determined to be based on the active sites Ser, Tyr, and Lys. Our work not only confirms that E. ludwigii YYP3 has promising application prospects in large-scale production of BHMF, but also provides novel insights into understanding the molecular mechanism of HMF reduction.
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TALANTA
·
2022
·
IF 6.556
Hao Feng,Fan Wang,Junhua Li,Qian Wu,Ying Cui,Lingzhi He,Xing Liu,Zeng Liu,Dong Qian,Haixia Tong
Lack of highly efficient, inexpensive, and easily available catalysts severely limits the practical applicability of electrochemically sensing assay towards 5-hydroxytryptamine (5-HT). Herein, four kinds of Fe–Co bimetallic Prussian blue analogues (FeCo–PBAs) with different molar ratios of Fe to Co were prepared using a simple coprecipitation method. Interestingly, Fe(III) in K 3 [Fe(CN) 6 ] can be reduced to Fe(II) by adding trisodium citrate dehydrate, which could offer a new clue to synthesize PBAs with Fe(II) core ions. With the optimizational FeCo-PBA synthesized at a 0.5/1 M ratio of Fe to Co as an electrocatalyst , the constructed sensor shows excellent comprehensive performance for the 5-HT assay with a high sensitivity of 0.856 μA μM −1 and an ultralow detection limit of 8.4 nM. Under the optimum conditions, linearity was obtained in the ranges of 0.1–10.0 μM and 10.0–200.0 μM and preferable recoveries ranged from 97.8% to 103.0% with relative standard deviation (RSD) < 4.0%. The integrated properties of FeCo-PBA can be comparable to previously reported electrocatalysts for the 5-HT assay including noble metal-based and expensive carbon (graphene and carbon nanotubes)-based electrocatalysts. The proposed sensor also exhibits outstanding selectivity, reproducibility, and practicality for real sample analyses. This work is the first report on the PBA-based sensor for the 5-HT assay, verifying the practicability of this high-performance sensor for the 5-HT assay.
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PubMed
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PROGRESS IN ORGANIC COATINGS
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2022
·
IF 6.206
Liying Song,Zhan Gao,Qiang Sun,Guiwen Chu,Hao Shi,Ningjing Xu,Zhenxing Li,Nini Hao,Xiaoying Zhang,Fubin Ma,Lifei Wang
Hollow mesoporous silica microspheres (HMSN) were selected as carriers for storing 2-aminino-5-mercato-1,3,4-thiadizole (ATM) in this experiment. The synthesised microspheres were uniformly dispersed, with a diameter of approximately 500 nm, as identified by scanning electron microscopy. HMSN, as excellent nanocarriers, were used to encapsulate ATM with a 19 wt% loading rate. Then, 18 wt% HMSN loaded with ATM was added to the coating. Electrochemical impedance spectroscopy and scanning Kelvin probes were used to investigate the self-healing ability of the coating with ATM encapsulated in hollow mesoporous silica microspheres. The copper corrosion caused by microdefects in the coating was delayed by controlling the slow release of ATM from the microspheres. The active corrosion resistance of the coatings was strengthened. By optimising the coating, the service life of the coating can be extended to achieve the long-term corrosion protection of copper.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2023
·
IF 4.3
Mu-Ying Guan,Chang-Ying Hu,Qi-Shan Peng,Ying Zeng,Wen-Wei A.,Ze-Chun Wu,Zhi-Wei Wang,Huai-Ning Zhong
Bamboo sticks intended for food contact can produce 5-Hydroxymethylfurfural (5-HMF) and Furfural (FF) when used in high-temperature scenarios (e.g., barbecue and Kanto boil). The influencing factors in terms of baking conditions, salinity, pH, and dipping time of water on the formation of 5-HMF and FF in bamboo sticks were investigated. Specific migration of 5-HMF and FF also have been studied in bamboo sticks in contact with food simulants (water, 10 % ethanol, and 4 % acetic acid). The results showed that the effects of baking temperature and time on the formation of both showed a similar pattern which firstly increased and decreased afterward. Both 5-HMF and FF levels in bamboo sticks increased with decreasing pH and the presence of salt. After dipping bamboo sticks in water for a while, the moisture content of higher than 10 % in bamboo sticks presented low levels of 5-HMF and FF. In the case of all food simulants, the highest migrated concentration of 5-HMF and FF were found in 4 % acetic acid. Since there are no specific migration limits for 5-HMF and FF, estimated daily intake is calculated to evaluate their safety. Based on the studied migration results, 5-HMF and FF in bamboo sticks are relatively safe for consumers.
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SURFACE & COATINGS TECHNOLOGY
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2022
·
IF 4.865
Juan Du,Zhaolin Wang,Ziming Wei,Jiawei Yao,Haipeng Song
This paper investigated the preparation of new environmental, pH stimulation response nanocontainer enhanced, self-healing, and efficient anti-corrosion coating for aluminum alloy protection. Silane/Ce-ZSM-5 coating with improved morphology was successfully synthesized on aluminum alloy surface, through the new proposed “hydrothermal crystallization - ion exchange - self-assembled seed growth - hot pressing” technology, in which ZSM-5 molecular sieve was served as pH stimulation response nanocontainer. The corrosion resistance and self-healing ability of the coating in 3.5 wt% NaCl solution were further investigated by the combined analysis of SEM, EIS, LEIS , ICP-MS characterization and 3D microscopic observation. The experimental results showed that the prepared silane-Ce-ZSM-5 coatings exhibited excellent corrosion protection and self-healing ability, which was attributed to the pH stimulation release of corrosion inhibitor Ce 3+ when the coatings were damaged. The ZSM-5 zeolites generated Ce(OH) 3 or CeO 2 precipitates to gradually fill the aluminum alloy defects, thus forming a dense protective layer and inhibiting the corrosion activity.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Xinyi Xing,Ying Guan,Liping Zhang,Xian Shi,Han Wu,Hui Gao,Siquan Xu
A catalytic system that is both efficient and recyclable is desirable for production 5-hydroxymethylfurfural (HMF) from glucose. In this study, the catalytic system composed of H 2 O (NaCl) -tetrahydrofuran (THF) biphasic system and H-β zeolite was found to have excellent performance for the glucose conversion into HMF. The physicochemical properties of the H-β zeolite catalyst, the dosage of the system components, and the reaction parameters were investigated in detail to optimize the production efficiency of HMF. Under optimal reaction conditions, an advanced level of 84% HMF yield was obtained from glucose. After the reaction was completed, all components of the catalytic system can be recovered, realizing no waste of reagents. Moreover, the recycled H-β(30) zeolite catalyst maintained considerable catalytic stability after five consecutive cycles. Therefore, it is reasonable to believe that the efficient, inexpensive, and recyclable H 2 O (NaCl) -THF catalytic system containing H-β(30) zeolite is capable of showing promising application potential in the future.
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FUEL
·
2022
·
IF 8.035
Shuai Wang,Thomas L. Eberhardt,Hui Pan
A lignin-derived mesoporous carbon solid acid catalyst (LDMCC) was prepared using alkali lignin as a carbon source and KCl as a salt template to generate a carbon support that was carboxylated with acrylic acid. The prepared LDMCCs were characterized by various spectroscopies (FTIR, XPS, XRD, Raman), porosity determinations (BET), microscopies (SEM, TEM), thermogravimetric analysis, and acid-base titration. The LDMCC produced at the highest carbonization temperature (900 °C) possesses a rich porous structure, high specific surface area (1197.1 m 2 ·g −1 ), large pore volume (0.63 cm 3 ·g −1 ), and abundant –COOH groups (2.4 mmol·g −1 ). This weakly acidic catalyst exhibits excellent synergistic catalytic performance with DMSO in the catalytic dehydration of fructose to prepare 5-hydroxymethylfurfural (5-HMF); the yield of 5-HMF was 96.0% using dimethyl sulfoxide as the solvent, reaction conditions of 180 °C for 2.0 h, and a catalyst loading of 0.1 mg·mg −1 . In addition, the prepared LDMCC exhibits excellent reusability over five cycles of use without significant loss in its catalytic activity. This study provides a novel green route for the preparation of a weakly acidic catalyst which may be useful for a variety of biomass conversion processes.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2022
·
IF 3.269
Guangyuan Chen,Yunhai Shi,Rongchun Shen,Wei Li,Jinghong Zhou
Two kinds of ketones , 5-methyl-2-hexanone and di-isobutyl ketone were selected as the extraction agents for separating the azeotrope of ethylene glycol (EG)and 1,2-butanediol (1,2-BDO). By comparing the results of preliminary extraction experiments under 303.15 K and normal pressure, 5-methyl-2-hexanone was the better one. And the Liquid-liquid equilibrium data of EG + 1,2-BDO + 5-methyl-2-hexanone ternary system were successively measured at 293.15 K and 313.15 K. The distribution coefficient ( K 2 ) and selectivity coefficient ( S ) of 1,2-BDO were calculated from the experimental data. The LLE data were correlated by NRTL and UNIQUAC activity models with the authorized Aspen Plus software. The root mean square deviations ( RD ) between the experimental and calculated values were all less than 0.7%, which means they were consistent with each other very well.
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TALANTA
·
2022
·
IF 6.556
Jin Wang,Lin Zhou,Jiali Bei,Qiyuan Zhao,Xue Li,Jiaqi He,Yan Cai,Tingting Chen,Yukou Du,Yong Yao
Pillar [5]arene, a new water-soluble carboxylatopillar [5]arene ammonium salts (WP5), has been employed as the host for complexation of guest molecules. Herein, a visible light driven WP5 functionalized gold nanoparticles (Au@WP5) was fabricated for ultrasensitive photelectrochemical (PEC) detection of caffeic acid (CA). The ultraviolet–visible spectrum characteristics, PEC response results of samples in caffeic acid solution confirm the localized surface plasmon resonance effect of Au NPs and the host-guest interaction between WP5 and CA are responsible for the enhanced PEC sensing performance. Under optimal conditions, the sensitive PEC sensor constructed with Au@WP5 exhibited the concentration linear range from 0.025 μM to 370 μM and a detection limit of 0.01 μM (S/N = 3). Importantly, the good anti-interference ability, stability and reproducibility of the proposed PEC sensor providing the promising detection application of pillar [5]arene functionalized photoactive materials in food and drinks.
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Reaction Chemistry & Engineering
·
2022
·Vol. 7
·期 8
·1742-1749
·
IF 5.2
Chaoqiang Wu,Chengyong Wang,Alei Zhang,Kequan Chen,Fei Cao,Pingkai Ouyang
3-Acetamido-5-acetylfuran (3A5AF) is an important platform compound, possessing very promising application prospects. Herein, we propose a new approach to convert N-acetylglucosamine (NAG) and chitin to 3A5AF using biobased deep eutectic solvents (DESs) containing choline chloride and various organic acids or polyols. A comparison of catalytic capacity showed that a DES made with choline chloride/citric acid (CCCA) possesses the optimum catalytic properties, which lead to a maximum yield for 3A5AF of 47.1 mol% and 5.0 mol% from NAG and chitin, respectively, at 210 °C in N,N-dimethylacetamide solvent with CaCl2·2H2O as an additive. Moreover, CCCA showed excellent recyclability and retained over 63.6% of its original activity after five cycles of use. In addition, the 3A5AF product was obtained with 99.0% purity by simple extraction and crystallization. This research provided a new avenue for 3A5AF production from renewable chitin resources.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Guoqiang Hou,Tingjun Fu,Xin Li,Qian Ma,Zhong Li
HZSM-5 catalysts with abundant silanol nests were fabricated by removing framework Al, which effectively promoted the selective alkylation of toluene with methanol by inhibiting the deep alkylation of aromatics to heavy aromatics and the conversion of methanol to light hydrocarbons. Correspondingly, the alkylation efficiency reached 65.3% at a toluene conversion of 31.3% over dealuminated HZSM-5, higher than the 55.2% efficiency and 28.0% conversion of parent zeolites, respectively. In situ DRIFTS and single-factor experimental clarified that toluene adsorption was enhanced and methanol to hydrocarbons was inhibited with the presence of silanol nests. Additionally, by increasing the crystal size of HZSM-5 with silanol nests from 2 to 5 µm, para-xylene selectivity was increased from 36.1% to 65.5% because of the enhanced diffusion barrier . The finding of the positive effect of the silanol nests on toluene alkylation can provide a solid fundamental basis for the rational design of catalysts.
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DIGESTIVE DISEASES AND SCIENCES
·
2022
·Vol. 68
·期 3
·778-790
·
IF 3.487
Gu Dan,Cao Ting,Yi Shijie,Liu Ya,Fan Chao
Background Ulcerative colitis (UC) features chronic, non-infectious inflammation of the colon. Insulin-like growth factor binding protein 5 (IGFBP5) has been indicated to be related to various inflammation-related diseases. However, its association with UC remains largely unclear. Aims Here, we investigate the role of IGFBP5 in colonic mucosal epithelial cell injury in UC. Methods Differentially expressed genes in the colonic tissues of UC mice were screened using the Gene Expression Omnibus database, and IGFBP5 was identified. UC mice were developed using dextran sulfate sodium, and IGFBP5 expression in the colonic tissues of UC mice was confirmed by immunohistochemistry and RT-qPCR. The effects of IGFBP 5 in vivo and in vitro were investigated by intraperitoneal injection of adeno-associated virus into UC mice or by transfection with an IGFBP5 overexpression plasmid into lipopolysaccharide-treated colonic mucosal epithelial cells. The mechanisms causing IGFBP5 deletion in UC were predicted by bioinformatics analysis and ChIP-qPCR and verified by rescue experiments. Results IGFBP5 was reduced in UC. IGFBP5 impaired the NFκB pathway in the colonic tissue of UC mice and ameliorated inflammatory infiltration and colonic mucosal cell injury. IGFBP5 depletion was associated with H3K27me3 modification, which was induced by EZH2. CTCF was responsible for recruiting EZH2 to the promoter region of IGFBP5. CTCF inhibition repressed UC progression by reducing H3K27me3 modification via the discouragement of the enrichment of EZH2 in the IGFBP5 promoter. Conclusions CTCF modulates H3K27me3 modification of the IGFBP5 promoter by recruiting EZH2, thereby downregulating IGFBP5 to accentuate colonic mucosal epithelial cell injury in UC mice.
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