APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
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2013
·Vol. 171
·期 7
·1559-1567
·
IF 1.893
Wang Na,Zhang Wei,Zhou Long-Hua,Deng Qing-Feng,Xie Zong-Bo,Yu Xiao-Qi
A facile tandem route to α,β-unsaturated aldehydes was developed by combining the two catalytic activities of the same enzyme in a one-pot strategy for the aldol reaction and in situ generation of acetaldehyde. Lipase from Mucor miehei was found to have conventional and promiscuous catalytic activities for the hydrolysis of vinyl acetate and aldol condensation with in situ formed acetaldehyde. The first reaction continuously provided material for the second reaction, which effectively reduced the volatilization loss, oxidation, and polymerization of acetaldehyde, as well as avoided a negative effect on the enzyme of excessive amounts of acetaldehyde. After optimizing the process, several substrates participated in the reaction and provided the target products in moderate to high yields using this single lipase-catalyzed one-pot biotransformation.
研究领域:
生物化学
·
酶工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2019
·
IF 2.931
Wenzhi Xu,Xue Li,Mengnan Han,Tingting Zhou,Yutao Yang,Wei Li
Hydrazine is extremely harmful to the human body. The leakage of hydrazine is liable to cause potential safety hazards. Here, we reported a new fluorescence probe based on the tandem reaction . The hydrazine-triggered hydrazinolysis-cyclization resulted in the formation of the iminocoumarin. The fluorescence intensity at 522 nm of the probe increased after the reaction with hydrazine. There was a linear relationship between the fluorescence intensity and the concentration of hydrazine (0.14–120.00 μM). The LOD of the probe to N 2 H 4 was 1.36 ppb. Notably, the probe could detect hydrazine in BT474 cells and tap water.
研究领域:
分析化学
·
环境科学
·
生物医学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Jie Liu,Jianhao Cui,Lei Chen,Jingjing Chen,Huidong Zheng,S. Ted Oyama
The conversion of terpinolene epoxide to terpinen-4-ol is a desirable chemical transformation for the production of a valuable intermediate. This paper describes a one-pot, two-step system for the reaction that uses a bifunctional Ni/TiO 2 -SiO 2 catalyst with isomerization and hydrogenation capabilities. The TiO 2 -SiO 2 serves to isomerize the starting epoxide. The Ni component works to hydrogenate the allylic double bond. The tandem system achieves a high 64% yield of terpinen-4-ol. X-ray diffraction analysis showed that TiO 2 -SiO 2 was a mixed binary oxide, and Fourier transform infrared spectroscopy of adsorbed pyridine suggested that acid sites were mainly Lewis acid sites. Electron microscopy showed that the Ni/TiO 2 -SiO 2 catalyst consisted of spherical particles comprising a titanosilicate phase with highly dispersed zero-valent Ni or anatase on the surface. Additionally, there was strong interaction between Ni and the TiO 2 -SiO 2 mixed oxides. Control kinetic experiments demonstrated that the tandem use of the catalysts was more effective than simultaneous operation.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Wei Liu,Yu-Qing Zhang,Zhen-Lin Dong,Zi-Xuan Chen,Lei Li,Xin-Yuan Zhao,Yang Wu,Yu-Yang Zhang
Graphical Here, the core-shell structure of ZIF-90@ZIF-67 was applied for the first time to catalyze the tandem reaction in Pickering emulsion system, which exhibited excellent catalytic performance with 99.9 % yield. Furthermore, ZIF-90@ZIF-67 has high stability and maintains good reproducibility after five cycles. This work provides a platform for the design of structurally and functionally diverse MOF-based interfacial catalysis for Pickering emulsions. Exploiting advanced solid particles is crucial to the construction of Pickering emulsions catalysis. Recently, metal-organic frameworks (MOFs) have been used as ideal emulsifiers stabilizing Pickering emulsions for interfacial catalysis. Although Pickering emulsions stabilized by core-shell MOFs have significant importance in practical studies, to date there have been very limited reports on this topic. Herein, ZIF-90@ZIF-67, a core-shell material with simultaneous acid-base bifunctionality, was synthesized by seeded epitaxial growth. It was firstly applied as an emulsifier in Pickering emulsions to catalyze the deacetalization-Knoevenagel tandem reaction, which exhibited excellent catalytic properties and achieved extremely high yields. Additionally, ZIF-90@ZIF-67 showed high stability and remained well repeatable after five cycles. This work provides a platform for the design of structurally and functionally diverse MOF-based Pickering emulsions interfacial catalysis.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
·
2013
·Vol. 2013
·期 32
·7411-7420
·
IF 3.344
Zhengkai Chen,Weijun Yang,Lijun Xu,Lili Zhang,Maozhong Miao,Hongjun Ren
Graphical Highly substituted 2-hydroxyflavanones can be obtained through a tandem O -arylation/hydroxylation process from triazenylaryl-substituted diketones in the presence of a Lewis acid. A transition-metal-free tandem O -arylation/hydroxylation approach has been developed for the efficient synthesis of highly substituted 2-hydroxyflavanones from triazenylaryl-substituted diketones. The intermediate benzopyrylium cation may be involved in these reactions.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Jing Wang,Tianqinji Qi,Zhibin Li,Wei She,Xuewei Li,Jingfang Li,Pengfei Yan,Weizuo Li,Guangming Li
Three novel N-doped carbon supported Co/Co 3 O 4 catalysts, namely, Co@CN- hmta , Co@CN- larg and Co-Co 3 O 4 @CN- bipy , with sheet-, worm-, honeycomb-like morphologies respectively, have been fabricated by the pyrolysis of well-defined coordination polymers (CPs). Upon the as-prepared catalysts were applied for the reaction of N-alkylation of nitroarenes with ethanol, a direct two-step tandem reaction is realized, in which the Co@CN- hmta delivers 100% conversion/selectivity of N-ethylaniline/N , N-diethylaniline from the direct N-alkylation of nitroarenes with ethanol. The kinetic studies were conducted to confirm that the N-alkylation of aniline with ethanol is the rate-determining step in the two-step tandem reaction. The SEM/EDX, XRD, Raman, TEM, XPS, and CO 2 -TPD characterization results have revealed that sizes and dispersion of metallic Co, amount of structural defects and surface Lewis basicity towards three catalysts can be tuned by changing the structures of Co-based CPs designed by different organic linkers, which may also help to understand the preparation of industrial catalysts on a molecular level. The optimized Co@CN- hmta catalyst is easily recycled by using the external magnet for successive reuses without any loss in both activity and selectivity. To the best of our knowledge, this is the first carbon-nitrogen species supported Co/Co 3 O 4 catalysts derived from the CPs, which could effectively catalyzed the N-alkylation of nitroarenes with ethanol to produce the secondary amines and/or tertiary amines. This low-cost, recyclable and easy scale-up N-doped carbon supported catalyst may be of potential application in various heterogeneous catalytic reactions.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 1
·143
·
IF 3.9
Yong Tang,Ciduo Wang,Hanqing Xie,Yuelin Xu,Chunyu Wang,Chuang Du,Zhi Wang,Lei Wang
The development of non-natural enzymatic catalysis is important for multicomponent tandem organic transformations. However, the delicate acting environments of biological enzymes still present some challenges in the synthesis of spirooxindole skeleton via enzymatic catalysis. To address these issues, a lipase-catalyzed method was developed for the synthesis of spirooxindole frameworks. Using easily available isatins, cycloketones, and malononitriles as substrates, mild reaction conditions, and a reasonable reaction time, moderate to good yields (67–92%) and excellent functional group tolerance were accomplished via this protocol. The related mechanism explanation is also speculated in this paper.Keywords:spirooxindoles;lipase catalysis;one-pot tandem process;green synthesis
研究领域:
有机化学
·
生物催化
✓ 已验证
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 18
·14235-14245
·
IF 4.6
Tong Su,Daguo Wu,Xinghua Zhang,Qi Zhang,Lungang Chen,Xiuzheng Zhuang,Longlong Ma
Biomass is an important renewable resource in nature, and cellulose is a crucial component within it. The chemically directed conversion of cellulose into ethylene glycol offers a green alternative to traditional petroleum-based production methods. In this study, a multifunctional Ni–WOx/SAPO-11 catalyst was designed. By optimizing the processing parameters of catalysts and the reaction conditions of them, it was demonstrated that this catalyst could efficiently catalyze cellulose into alcohol products through a series of tandem reactions such as hydrolysis, retro-aldol condensation, and hydrogenation under relatively mild conditions. The yield of ethylene glycol climbed from 4% (at 180 °C) to 66.6% (at 240 °C) with the increase of reaction temperature. Characterization (XPS, TEM, TPD/TPR) revealed that a reduction temperature of 500 °C maximized Brønsted acidity and W5+/W6+ ratios, enhancing C–C cleavage efficiency. Further increases in the reduction temperature would weaken the Brønsted acid on the surface of SAPO-11, but its surface area would also increase (mainly in the form of mesopores). The uniformly dispersed elemental tungsten could form new acidic sites on the catalyst surface; in combination with active Ni0, this high-temperature reduced catalyst could achieve the direct hydrogenolysis of cellulose to produce ethylene glycol, benefiting the efficient utilization of lignocellulosic biomass in the future.
研究领域:
生物质能
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催化化学
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Yuefeng Qiu,Peng Jiang,Wenkai Ye,Jiahao Hu,Bin Zhang,Tuo Ji,Liwen Mu,Xin Feng,Xiaohua Lu,Jiahua Zhu
An electrochemical–thermal tandem reaction system was designed in this work and enabled the highly efficient synthesis of propylene oxide (PO) at 1 atm without the use of H2O2. The electrochemical part produced OOH− through a 2e− oxygen reduction reaction, which migrated and distributed in the full space of a chamber filled with a mixture of solid electrolyte particles and modified TS-1 (m-TS-1) catalysts. Mediated by the relay of OOH− and protic solvent methanol, full space tandem reactions were achieved with a high PO selectivity of 95.2% and a productivity of 319.75 mmol gecat−1 h−1. A mechanistic study revealed that the m-TS-1 catalysts accepted the migrated OOH− and formed a Ti-OOH intermediate, which played a key role in relaying the tandem reactions for an efficient propylene epoxidation reaction. Techno-economic analysis and life-cycle assessment revealed favorable figures for the proposed process compared to the conventional process.
研究领域:
化学工程
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催化科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Chemistry of Heterocyclic Compounds
·
2014
·Vol. 50
·期 1
·12-18
·
IF 0.698
Ge H. Y.,Fang Z. J.,Qian B. H.
3-Arylcoumarins were conveniently synthesized in excellent yields by an iron(III) chloride-promoted tandem reaction using methoxy-substituted ( E )-2,3-diphenylpropenoic acids or their methyl esters. The structure of 3-(4-methoxyphenyl)coumarin was established from X-ray crystallographic data.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Ying Zhang,Jie Qi,Hongsheng Lu
To accommodate the advancement of green chemistry and further enhance hydrogen utilization efficiency and organic compound conversion in reactions, a smart Pickering emulsion stabilized by modified Janus silica particles was successfully prepared for the tandem reaction of ammonia borane hydrolysis and organic hydrogenation reduction. The emulsion has been confirmed to possess high stability and rapid stimulus responsiveness. The high stability and large oil-water interface area of Pickering emulsions, along with their low energy demulsification method, provide an excellent reaction platform and catalyst in situ recovery strategy for tandem reactions. Moreover, the anisotropy of Janus particles facilitates the progression of tandem reactions, mitigating the waste associated with "sacrifice" mechanisms and averting hydrogen loss. Experimental results demonstrate that even when the molar amount of hydrogen released from ammonia borane is comparable to that of organic compounds, organic compounds still achieve a conversion rate of 99 %, with a hydrogen utilization efficiency 3–4 times higher than that of conventional two-phase systems. By simply adjusting the pH, the catalyst can be recovered in situ for the next cycle. Even after 5 cycles, a high conversion rate of organic compounds is maintained.
研究领域:
绿色化学
·
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
STEROIDS
·
2013
·
IF 2.803
Shu-Xiao Feng,Ya-Dong Zhang
One-pot synthesis of an 18-norsteroid compound, 13( R ),14( R )-epoxy-17β-methyl-20( S )-hydroxyl-18-nor-pregna-4-en-3-one has been achieved with peracetic acid/acetic acid under a mild condition, via a proved tandem epoxidation-rearrangement-epoxidation sequence. Its structure was designated on the basis of NMR and X-ray crystallography data.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）