GREEN CHEMISTRY
·
2019
·Vol. 21
·期 16
·4434-4442
·
IF 9.405
Teng Li,Shengqin Liu,Bing Wang,Jingen Long,Jun Jiang,Ping Jin,Yao Fu,Haizhu Yu,Weiran Yang
Glycerol, generated in abundance as the by-product in the process of biodiesel production and saponification, has seen attempts to convert it into value-added chemicals. However, due to the low selectivity of hydrogenolysis of the secondary hydroxyl group, valuable 1,3-substituted chemicals are difficult to obtain from glycerol by chemocatalysis. In this work, glyceric acid (GA), a renewable biomass from glycerol, was quantitatively converted to 3-iodopropionic acid (3-IPA) at 373 K in 3 h by hydroiodic acid mediated hydrogenation. As the reductant in this process, HI is oxidized to I2 and then regenerated in situ by metal catalysts and H2. The reaction pathway was proposed by intermediate identification and verified by a kinetics study and computational method. The catalytic system was shown to be stable and can be reused several times without loss in activity. As a 1,3-substituted chemical, 3-IPA is not only a potential monomer to form poly-3-hydroxypropionic acid, but also a good platform molecule to produce useful chemicals, e.g. 3-hydroxypropionic acid (3-HPA) and acrylic acid (AA), due to its highly reactive nature.
研究领域:
化学工程
·
可再生资源化学
·
有机合成
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·Vol. 29
·期 52
·e202300950
·
IF 4.3
Fukun Li,Ronghe Yang,Zheng Tian,Ziting Du,Jinhang Dai,Xingmin Wang,Ning Li,Jie Zhang
Graphical Microwave-assisted one pot cascade transformation of furfural to γ-valerolactone catalyzed by Sc(OTf) 3 . γ-Valerolactone (GVL) is considered as a star biochemical which can be used as a green solvent, fuel additive and versatile organic intermediate. In this study, metal triflate (M(OTf) n ) was utilized as the catalyst for one-pot transformation of furfural (FF) to GVL in alcohol media under microwave irradiation. Alcohol plays multiple functions including solvent, hydrogen donor and alcoholysis reagent in this cascade reaction process. And process efficiency of GVL production from FF upgrading is strongly related to the effective charge density of selected catalyst and the reduction potential of selected alcohol. Complex (OTf) n -M−O(H)R, presenting both Brønsted acid and Lewis acid, is the real catalytic active species in this cascade reaction process. Among various catalysts, Sc(OTf) 3 exhibited the best catalytic activity for GVL production. Various reaction parameters including the Sc(OTf) 3 amount, reaction temperature and time were optimized by the response surface methodology with the central composite design (RSM-CCD). Up to 81.2 % GVL yield and 100 % FF conversion were achieved at 143.9 °C after 8.1 h in the presence of 0.16 mmol catalyst. This catalyst exhibits high reusability and can be regenerated by oxidative degradation of humins. In addition, a plausible cascade reaction network was proposed based on the distribution of product.
研究领域:
化学工程
·
生物化工
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Le Gao,Yawen Li,Guifang Li,Jiaqi Huo,Lishan Jia
Interface engineering as an effective material modification method can regulate local corresponding interfacial geometry and electronic structures, thus enabling a higher intrinsic activity for the oxygen evolution reaction (OER). Herein, we carefully designed p-p heterojunction precursor Co4-MOF@La(HCO 2 ) 3 with internal electric field through electrostatic adherence, which then in-situ transformed into p-p type heterojunction electrocatalyst (Co(OH) 2 )4@La(OH) 3 under KOH activation strategy. The one-step in-situ conversion of (Co(OH) 2 )4@La(OH) 3 generated the interface with significant difference in metal atomic radius and exhibits fascinating nanostructures, which enhances the specific surface area and increases the number of active sites compared with the parent material. Impressively, the obtained material (Co(OH) 2 )4@La(OH) 3 demonstrates satisfying electrocatalytic activity in OER with a low overpotential of only 233 mV to reach a current density of 20 mA cm −2 , and excellent stability for 50 h at 10 mA cm −2 in alkaline medium. In-situ Raman technique indicates that multivalent Co centers are the true active sites during the OER process. Based on density functional theory (DFT) calculation results, La atoms possess empty d orbitals, which are beneficial to facilitate charge transfer from Co to La at the heterojunction interface. Meanwhile, the introduction of La atoms changes the coordinated environment around the adjacent atoms at the interface, which induces the upshift of the d-band center for Co atoms and increases the binding strength of the adsorbed oxygen intermediate.
研究领域:
材料科学
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电化学
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能源转换与存储
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产品关联
DOI
高影响因子
TETRAHEDRON
·
2017
·
IF 2.651
Bing Lin,Wen-Hui Zhang,Dan-Dan Wang,Yi Gong,Qi-Di Wei,Xiong-Li Liu,Ting-Ting Feng,Ying Zhou,Wei-Cheng Yuan
Developed herein is a diversity-oriented one-pot multicomponent synthesis of polycyclic 3,3′- pyrrolidinyl-dispirooxindoles 3 via a multicomponent 1,3-dipolar cycloaddition event of 3-methyl-4-nitro-5-isatylidenyl-isoxazoles 2 with azomethine ylides (thermally generated in situ from isatins and proline or thioproline). Products bearing four consecutive stereocenters consist of two oxindole moieties and a polycyclic pyrrolidinyl core, including vicinal spiroquaternary stereocenters fused in one ring structure were smoothly obtained in high yields (up to 85% yield) with good diastereoselectivity (up to >20:1). Valuable features of this method were application of 3-methyl-4-nitro-5-isatylidenyl-isoxazoles as 1,3-dipolarophiles and the design of new hybrid architectures for biological screenings through the adequate fusion of these sub-units of isoxazole and 3,3′-pyrrolidinyl-dispirooxindole, generating drug-like molecules.
研究领域:
有机化学
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药物化学
·
肿瘤学
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产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2021
·
IF 7.514
Di Wu,Ran Duan,Lan Tang,Xia Hu,Fang Geng,Qiaomei Sun,Yin Zhang,Hui Li
The interaction between lipase and quercetin 3-rhamnoside was studied by fluorescence spectroscopy, enzyme kinetics, and molecular dynamics simulation. The results showed that quercetin 3-rhamnoside had a strong quenching effect on the intrinsic fluorescence of lipase. The binding constant decreased with increasing temperature, and the number of binding sites approached 1. Thermodynamic parameters indicated that hydrogen bonding and van der Waals forces are the dominant forces when the interaction occurs. Circular dichroism spectroscopy and infrared spectroscopy proved that the ligand perturbed the structure of lipase. Enzyme kinetics results showed that quercetin 3-rhamnoside inhibited lipase, and the inhibitory effect was dose-dependent. Molecular dynamics simulation further explained the interaction mechanism and inhibitory effect. This study confirmed the inhibitory effect of quercetin 3-rhamnoside on lipase explained their binding mechanism, which will contribute to guiding the development of fat-reducing functional foods.
研究领域:
生物化学
·
营养学
·
药理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2016
·Vol. 51
·期 24
·10849-10862
·
IF 2.302
Zhang Man,Li Chuan,Gao Huiqi,Fu Wei,Li Yingying,Tang Liwei,Zhou Zhiming
Twelve salts of 3-nitro-1,2,4-triazol-5-one (NTO) (ammonium, hydrazinium, guanidinium, aminoguanidinium, diaminoguanidinium, triaminoguanidinium, N -carbamoylguanidinium, semicarbazidium, 1,5-diamino-1,2,4-tetrazolium, 3,4,5- triamino-1,2,4-triazolium, 3,6,7-triamino-7H-[1, 2, 4]triazolo[5,1-c][1,2,4]triazol-2- ium, and 4,4′,5,5′-tetraamino-3,3′-bi-1,2,4-triazolium) were synthesized. The new salts were fully characterized by 1 H and 13 C NMR spectroscopy, infrared spectroscopy, and elemental analysis. The crystal structures of salts 10 and 11 were determined by single-crystal X-ray diffraction. All energetic salts except salt 6 exhibit excellent thermal stabilities with decomposition temperatures ranging from 203 to 270 °C. The densities of salts ranged from 1.65 to 1.88 g cm −1 as measured by a gas pycnometer. Theoretical performance calculations (Gaussian 03 and EXPLO5 v6.01) yielded detonation pressures and detonation velocities for the energetic salts, ranging from 24.4 to 38.1 GPa and 8136 to 9575 m s −1 , respectively. In particular, salt 2 has an outstanding detonation performance ( P
cj = 38.1 GPa, v
D = 9575 m s −1 ) with a satisfactory acidity compared to that of NTO ( pK
a = 5.63 versus pK
a = 2.37). Furthermore, the particles of salt 2 form two-dimensional blades of submicron size, as determined by scanning electron microscopy analysis. Meanwhile, salt 2 was compatible with TNAZ, TATB, TKX-50, Al, NH 4 ClO 4 , CL-20, TNT, and F2603 fluororubber, as determined by differential scanning calorimetry or vacuum stability tests.
研究领域:
化学
·
材料科学
·
爆炸物研究
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产品关联
DOI
高影响因子
iScience
·
2024
·
IF 4.6
Ruobing Wang,Dan Su,Yueze Liu,Hua Huang,Jiangdong Qiu,Zhe Cao,Gang Yang,Hao Chen,Wenhao Luo,Jinxin Tao,Guihu Weng,Taiping Zhang
Summary Nuclear factor kappa B (NF-κB) plays a pivotal role in the development of pancreatic cancer, and its phosphorylation has previously been linked to the regulation of NUAK2. However, the regulatory connection between NF-κB and NUAK2, as well as NUAK2’s role in pancreatic cancer, remains unclear. In this study, we observed that inhibiting NUAK2 impeded the proliferation, migration, and invasion of pancreatic cancer cells while triggering apoptosis. NUAK2 overexpression partially resisted apoptosis and reversed the inhibitory effects of the NF-κB inhibitor. NF-κB transcriptionally regulated NUAK2 transcription by binding to the promoter region of NUAK2. Mechanistically, NUAK2 knockdown remarkably reduced the expression levels of p -SMAD2/3 and SMAD2/3, resulting in decreased nuclear translocation of SMAD4. In SMAD4-negative cells, NUAK2 knockdown impacted FAK signaling by downregulating SMAD2/3. Moreover, NUAK2 knockdown heightened the sensitivity of pancreatic cancer cells to gemcitabine, suggesting that NUAK2 inhibitors could be a promising strategy for pancreatic cancer treatment.
研究领域:
肿瘤学
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分子生物学
·
细胞生物学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 50
·31601-31607
·
IF 3.361
Bi-Xian Zhang,Pei-Shan Li,Ying-Ying Wang,Jia-Jun Wang,Xiu-Lin Liu,Xue-Yang Wang,Xiao-Mei Hu
Indole-3-acetic acid (IAA) plays an important role in the growth and development of plants. In this study, a series of predominant strains were isolated and identified as Enterobacter sp. with remarkable IAA-producing capabilities. The IAA-producing strains are mainly tryptophan-dependent and have significantly high yields of IAA (3477 μg mL−1 and 3378 μg mL−1). The ipdC gene encoding indole-3-pyruvate decarboxylase was identified by genomic analysis and RT-qPCR analysis, indicating the involvement of the indole-3-pyruvic acid (IPyA) pathway of IAA biosynthesis. The IPyA pathway was also confirmed by the intermediate assay. The IAA product of microbial metabolites was isolated, purified and characterized. These microbes exhibiting IAA production significantly promoted the growth of maize, increasing root length, plant height, fresh weight and dry weight. Thus, Enterobacter sp. with high IAA production has great prospects in agricultural and industrial applications.
研究领域:
微生物学
·
植物学
·
农业科学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yu Fu,Fangbo Zhao,Yingzheng Liu,Ruiqi Li,Hongxu Chen,Liu Yang,Zhiguo Li,Mingcong Wu,Dan Wang
In this research, we introduce a novel and efficient approach for enhancing both the antibacterial efficacy and resistance to protein fouling of nanofiltration (NF) membranes, marking the first report of a method capable of concurrently addressing these critical membrane performance parameters. After traditional interface polymerization (IP), NF membranes were post-treated by the antibacterial N-(3-Aminopropyl)-imidazole (ANPI) which can be grafted on the membrane by its amino group reacting with rest acyl chloride in IP on the surface. After parameter optimization of the ANPI concentration, the modified membrane NF-12 demonstrated up to 99% antibacterial activity against two representative pathogens, Escherichia coli and Staphylococcus aureus . Except for this, due to the zwitterionic effect, the modified membrane achieved a remarkable 68.7% enhancement in water flux and the recovery rate of BSA cyclic pollution reached 97.5%. From mechanism analysis, it can be proposed that the post-grafted ANPI brought antibacterial properties to the NF membrane, which was able to kill bacteria attached to the membrane surfaces. Also, the imidazole protonation introduced positive charges to the NF membrane surface, mixing with negative charges produced by acyl chloride hydration, which produced the zwitterionic effect and facilitated the formation of a robust hydrophilic hydration layer, thereby significantly diminishing the adhesion of contaminants.
研究领域:
材料科学
·
环境工程
·
生物医学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yiting Liao,Lanzhen Peng,Xiaosong Zhou,Jin Luo,Limei Xu,Xiaomei Ning,Xiaoqin Zhou,Xunfu Zhou,Yueping Fang
Two major challenges in photocatalysis are the separation and utilization of photogenerated charge carriers that have limited their wider applications. To address these issues, significant studies have been devoted to the surface modification of photocatalysts. Herein, CdS nanorods were surface-modified by an ion-conducting LiTi 2 (PO 4 ) 3 (LTP) shell. This modification could accelerate the rapid separation and efficient utilization of photoinduced charge carriers. Therefore, CdS@LTP composite photocatalyst displayed a photocatalytic H 2 evolution rate of 26.01 mmol g −1 h −1 without any addition of cocatalysts in a Na 2 S/Na 2 SO 3 solution, which was over 6-fold compared to CdS, and showed improved stability. Furthermore, this shell can prevent the reverse reactions between H 2 and O 2 during photocatalytic water splitting. With the photo-deposition of Pt cocatalysts, CdS@LTP-Pt can achieve efficient overall water splitting with the highest H 2 generation rate (351 μmol g −1 h −1 ), which is 3.25 times higher than that of CdS-Pt. This study broadens the application of ionic conductor materials and provides a new way for the design of advanced photocatalysts for solar energy conversion.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
FOOD AND CHEMICAL TOXICOLOGY
·
2014
·
IF 2.61
Chang Li,Shao-Ping Nie,Yong-qiang Zhou,Ming-Yong Xie
3-monochoropropane-1, 2-diol (3-MCPD) esters from edible oils are considered to be a possible risk factor for adverse effects in human. In the present study, the exposure assessment of 3-MCPD esters to Chinese population was performed. A total of 143 edible oil and fat samples collected from Chinese markets were determined for the concentrations of 3-MCPD esters. The concentration data together with the data of fats consumed were analyzed by the point evaluation and probabilistic assessment for the exposure assessment. The point evaluation showed that the mean daily intake (DI) of 3-MCPD esters were lower than the value of provisional maximum tolerable daily intake (PMTDI) of 3-MCPD (2 µg/kg BW/d). The mean DI values in different age groups obtained from probabilistic assessment were similar to the results of the point evaluation. However, in high percentiles (95th, 97.5th, 99th), the DI values in all age groups were undesirably higher than the value of PMTDI. Overall, the children and adolescents exposed more to 3-MCPD esters than the adults. Uncertainty was also analyzed for the exposure assessment. Decreasing the level of 3-MCPD esters in edible oils and consuming less oil were top priority to minimize the risk of 3-MCPD esters.
研究领域:
食品安全
·
毒理学
·
营养学
✓ 已验证
DOI
高影响因子
AMB Express
·
2019
·Vol. 9
·期 1
·1-9
·
IF 2.226
Zhao Shuxue,Hu Chunhui,Guo Lizhong,Li Kuiran,Yu Hao
A 3-hydroxypyridine degrading bacterium, designated strain DW-1, was isolated from petroleum contaminated soil in Liao River China. 16S rRNA-based phylogenetic analysis indicates that strain DW-1 belongs to genus Agrobacterium. The optimal cultivation temperature and pH for strain DW-1 with 3-hydroxypyridine were 30 °C and 8.0, respectively. Under optimal conditions, strain DW-1 could completely degrade up to 1500 mg/L of 3-hydroxypyridine in 66 h. The 3-hydroxypyridine degradation pathway of strain DW-1 was suggested by HPLC and LC–MS analysis. The first reaction of 3-hydroxypyridine degradation in strain DW-1 was α-hydroxylation so that the major metabolite 2,5-dihydroxypyridine was produced, and then 2,5-dihydroxypyridine was transformed by a Fe2+-dependent dioxygenase to form N-formylmaleamic acid. N-Formylmaleamic acid will be transformed to maleic acid and fumaric acid through maleamic acid. This is the first report of the 3-hydroxypyridine degradation pathway and the utilization of 3-hydroxypyridine by a Agrobacterium sp. It may be potentially used for the bioremediation of environments polluted with 3-hydroxypyridine.
研究领域:
微生物学
·
环境科学
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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）