ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2014
·
IF 2.549
Kai Dong,Cheng H. Sun,Jian W. Song,Gai X. Wei,Si P. Pang
Synthesis of 2,6,8,12-tetraacetyl-2,4,6,8,10,12-hexaazaisowurtzitane (TAIW) by catalytic hydrogenolysis of 2,6,8,12-tetraacetyl-4,10-dibenzyl-2,4,6,8,10,12-hexaazaisowurtzitane (TADBIW), a key step for the synthesis of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW), has been first implemented under continuous flow conditions using the commercially available H-Cube Pro reactor. Several variables (i.e., reaction temperature, flow rate, and pressure) and the stability of the system have been investigated to optimize the operating conditions. The results show that a continuous flow system provides a better yield than a batch system. For instance, the yield is 99% at the optimized conditions, while the best yield from batch reactions is 92%. Continuous flow synthesis of TAIW has potential applications in improving the production technologies of HNIW for its many advantages over batch reactions.
研究领域:
化学合成
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Jiali Chen,Chen Huang,Yuqing Zhang,Liya Zhou,Li Ma,Lihui Wang,Yanjun Jiang,Yunting Liu
The conversion of racemic alcohols to enantiopure alcohols and amines is of significant importance yet presents considerable challenges. Herein, we achieved this goal by developing continuous-flow chemoenzymatic systems. In chemical module, a ruthenium (II)-N-heterocyclic carbene (Ru-NHC) catalyst immobilized on dendritic organosilica nanoparticle (DON) was prepared, which exhibited high activity and selectivity in the dehydrogenative oxidation of racemic alcohols to ketones. In enzymatic module, a ketoreductase and an amine dehydrogenase were individually co-immobilized with a cofactor-regenerating enzyme (glucose dehydrogenase) on DON for the enantioselective conversion of ketones to chiral alcohols and amines, respectively. The integration of the two modules in continuous-flow systems enabled the efficient chemoenzymatic deracemization and asymmetric amination of racemic alcohols (9 examples) with the maximum space-time yields of 6.8 and 5.8 g L -1 h -1 , respectively, underscoring the practical utility of the continuous-flow chemoenzymatic systems.
研究领域:
生物化学
·
有机化学
·
合成生物学
✓ 已验证
产品关联
DOI
高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2023
·
IF 3.4
Feng Xu,Zhiquan Chen,Lei Ni,Gang Fu,Jian Liu,Juncheng Jiang
In this work, the continuous flow nitration of naphthalene to 1-nitronaphthalene was systematically studied from the microreactor to mesoscale flow reactor and the safety issues during the reaction process were investigated. The effect of the molar ratio of nitric acid to naphthalene, residence time, reaction temperature, and sulfuric acid strength on the reaction process was comprehensively investigated in the microreactor. Under optimal conditions, the reaction yield could reach 94.96%. Due to the rapid exothermic characteristics of nitration, a quick heat transfer assessment was proposed to obtain the temperature profile during optimal conditions. It was found that the maximum overtemperature during the reaction was only 3.78 °C, which was consistent with the high yield under the optimal conditions. Then a scale-up of the microreactor to production was realized by a dimension-enlarging strategy. In the mesoscale flow reactor, the influence of volumetric flow rates was investigated. The annual output of the flow reactor could reach 2643 kg·a–1 while the highest overtemperature inside the reactor channel well exceeded 17.1 °C. In addition, a conventional semibatch experiment was carried out in the batch calorimeter RC1e to explore the reaction’s exothermic characteristics. Finally, the performances of the two reactors were compared, showing that the continuous flow reactor had more advantages than the batch reactor in economic benefit and inherent safety.
研究领域:
化学工程
·
安全科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Heyong Wang,Meiluan Wang,Guixiang Huang,Mingye Zhao,Yongzhen Peng,Ning Zhu,Zheng Fang,Yujing Hu,Kai Guo
Optically active ethyl ( R )-2-hydroxy-4-phenylbutanoate (( R )-HPBE), is a key component in the production of angiotensin-converting enzyme (ACE) inhibitors, which are essential for treating hypertension. However, the high cost of starting materials has been a barrier to the industrial synthesis of ( R )-HPBE. Herein, we have established for the first time a four-step enzymatic reaction in continuous flow for the efficient synthesis of ( R )-HPBE from inexpensive benzaldehyde and pyruvic acid. This route also overcomes the issues of chemical disequilibrium and incompatibility of reaction conditions that are common in multi-enzyme cascades. The immobilization methods for aldolase/ene-reductase/keto-reductase were developed, and the immobilized enzymes were initially used in three individual flow modules to produce ( R )-2-hydroxy-4-phenylbutanoic acid (( R )-HPB), achieving high space–time yields of 3103 g (OPBEA) L −1 d −1 , 1685 g (OPBE) L −1 d −1 and 1709 g ( R )-HPB L −1 d −1 respectively. Moreover, integrating three modules in continuous flow achieved a space–time yield of about 350 g ( R )-HPB L −1 d −1 after 108 h, and maintained high operational stability with a conversion of >99 % and a product ee of >99.9 % after 192 h. Subsequently, the ethyl esterification of ( R )-HPB as the fourth module for producing ( R )-HPBE obtained a high space–time yield of 2117 g ( R )-HPBE L −1 d −1 , marking a substantial 74.5-fold increase over the batch system.
研究领域:
生物化学
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制药工程
·
酶工程
✓ 已验证
DOI
高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2019
·
IF 3.327
Xin-peng Ma,Jin-sha Chen,Xiao-hua Du
Hymexazol is an efficient and low-toxicity soil fungicide. In this work, a fully continuous flow process for the synthesis of hymexazol has been developed. This process begins with combining ethyl acetoacetate and hydroxylamine hydrochloride to form a hydroxamic acid intermediate. The reaction solution is then quenched with concentrated hydrochloric acid to obtain the final product, hymexazol. Under the optimized process conditions, the total yield of the target product reached 86%. In addition, production was successfully scaled-up to a kilogram scale. The continuous flow method not only greatly decreases the reaction time but also significantly inhibits the side reactions.
研究领域:
化学工程
·
农药科学
✓ 已验证
DOI
高影响因子
Journal of Flow Chemistry
·
2018
·Vol. 8
·期 3
·129-138
·
IF 1.658
Li Xin,Liu Zhuang,Qi Hao,Fang Zheng,Huang Siyu,Miao Shanshan,Guo Kai
To reduce the cost and improve the efficiency for rifampicin preparation, a continuous flow synthesis of rifampicin starting from rifamycin S and tert -butylamine was studied in a microreactor. Two reaction steps and one purification step were coupled in a microreactor, and rifampicin was obtained with 67% overall yield. This method used 25% less 1-amino-4-methyl piperazine and got 16% higher overall yield without changing solvent and purification process between steps. This method has a good potential for further industrial application.
研究领域:
制药工程
·
有机化学
✓ 已验证
DOI
高影响因子
Reactions
·
2024
·Vol. 5
·期 4
·812-822
·
IF 2.2
Joseph Dean,Natalia Buckler Reinoso,Francesco Spiedo,Carola Romero Fernández,Bhaven Patel
Flow chemistry has shown significant versatility over the last two decades, offering advantages in efficiency, scalability, and sustainability. In this study, the continuous stirred tank reactor (CSTR) was used to optimise the synthesis of α-hydroxyphosphonates via the Pudovik reaction and their subsequent conversion to phosphates through the phospha-Brook rearrangement. The study highlights that using CSTRs allows for better control over reaction parameters, leading to reduced reaction times and improved yields compared to traditional batch methods. The optimised conditions successfully facilitated a range of organophosphates, including electron-rich and electron-poor derivatives, with high efficiency. Additionally, a one-pot tandem process combining the Pudovik reaction and the phospha-Brook rearrangement was developed, reducing reaction times to two hours while maintaining comparable yields. This work demonstrates the potential of CSTRs in flow chemistry for synthesising complex organophosphorus compounds, achieving higher reaction yields and shorter reaction times, highlighting the effectiveness of continuous flow methodologies.
研究领域:
有机化学
·
合成化学
·
流程优化
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Minglei Li,Yaheng Zhang,Jie Zhang,Min Peng,Liuming Yan,Zhiyong Tang,Qing Wu
Gas–liquid–solid (G–L–S) three-phase slug flow provides an efficient pathway to utilize solid catalysts in continuous flow and was adopted in the mesoporous graphite carbon nitride (mpg-C3N4)-catalyzed photoinduced electron/energy transfer reversible addition–fragmentation chain transfer (PET-RAFT) polymerization of methyl methacrylate (MMA) in this work. Kinetic studies and chain extension experiments illustrated the realization of reversible deactivation radical polymerization (RDRP) and the “easy to scale up” advantage of a continuous-flow reactor as compared to its batch counterpart. The light intensity played an important role on the PET-RAFT polymerization. An increasing amount of photocatalyst favored the monomer conversion within a limited range due to higher light blockage, and the monomer conversion reached a stable level at a lower catalyst concentration when higher light power was applied. When compared with fully continuous flow, the G–L–S slug flow was beneficial to the PET-RAFT polymerization due to the intensified swirling strength and narrower velocity field. Decreasing the gas-to-slurry ratio also led to narrower velocity distribution, which favored the polymerization as well. Moreover, the polymerization rates remained stable in multiple recycles, demonstrating that the present G–L–S slug flow was a reliable and easy processing approach for utilizing the solid catalyst.
研究领域:
化学工程
·
高分子化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2016
·
IF 2.567
Wei He,Zheng Fang,Qitao Tian,Weidong Shen,Kai Guo
In this study, a novel protocol consisting of peroxidatic reaction and epoxidation process was developed. Besides, a specific continuous extraction apparatus was also employed in the continuous flow synthesis process. Without additional purification, m-chloroperbenzoic acid (m-CPBA) generated in situ could react with cyclohexene, leading to high quality cyclohexene oxide. In the first stage, m-CPBA was obtained within a few seconds at room temperature by reacting m-chlorobenzoyl chloride with hydrogen peroxide, while cyclohexene oxide was prepared at 30 °C for 10 min in the following stage.
研究领域:
有机化学
·
化学工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Yuxiong,Zhang Yaoyu,Wang Xiaoqiang,Liu Yue,Wu Zhongbiao
Photocatalytic direct oxidation of methane to C 1 oxygenates offers a green alternative to conventional energy-intensive and high-carbon-footprint multi-step processes. However, current batch-type gas–liquid–solid reaction systems under high-pressure conditions face critical challenges in real-time product separation and concentration for industrial implementation. Here, we demonstrate a continuous-flow gas – solid photothermal catalytic route for methane conversion to formaldehyde under ambient pressure, where the generated gas-phase formaldehyde can be easily collected by water absorption. The Ag single-atom modified ZnO photocatalyst achieves a formaldehyde production rate of 117.8 ± 1.7 μmol h −1 with 71.2 ± 0.8% selectivity. Meanwhile, a highly concentrated formaldehyde solution (514.2 ± 33.7 µmol mL −1 , 1.54 ± 0.10 wt.%) is obtained through 12-hour water absorption, effectively overcoming the product enrichment barrier that plagues conventional batch reaction route. This study establishes a robust technological foundation for sustainable industrial-scale conversion of methane to value-added chemicals.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Pengyu Yuan,Qing Wang,Xuelei Deng,Xiaoyan Zhang,Daidi Fan,Yunpeng Bai
Enzyme catalysis is a promising method for producing chiral chemicals with high stereoselectivity under mild conditions. However, the traditional batch reaction suffers from low enzyme stability, low cofactor recycling, and poor enzyme reusability. Here, we present a continuous-flow method using coimmobilized dual enzymes for the synthesis of chiral γ-/δ-lactones, which are widely used in fragrances and flavors. Typically, a carbonyl reductase mutant SmCRM5 from Serratia marcescens, was coimmobilized by covalent binding with BmGDH, a glucose dehydrogenase capable of recovering and recycling the cofactor NADPH. After immobilization, SmCRM5 and BmGDH exhibited a 8.9-/8.7-fold increase in catalytic efficiency (kcat/Km) and a 57-/15-fold increase in half-life at 30 °C, respectively. We demonstrated that coimmobilized dual enzymes used in a continuous flow reactor showed a higher reaction rate and a higher space-time yield (1586 g·L–1 d–1) than free enzymes and immobilized enzymes in a batch reaction for the production of (R)-δ-decalactone. This continuous flow reactor can run continuously for more than 650 h with 99% ee and 80% conversion, and the total volume exceeds 1500 reactor volumes. The robustness of this continuous-flow immobilized enzyme system provides a green and efficient method for the synthesis of high value-added chiral chemicals.
研究领域:
生物催化
·
酶工程
·
绿色化学
✓ 已验证
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Jinpei Huang,Yuhao Geng,Yundong Wang,Jianhong Xu
Cyclopropylamine (CPA) is an essential intermediate in the preparation of many biologically active substances. The traditional batch method to prepare CPA is facing many problems in the Hofmann rearrangement step, such as low production efficiency, poor stability, and complex process. In this paper, a novel continuous-flow method was developed to prepare CPA with high efficiency. Taking advantages of characteristics of the continuous-flow microreaction system, the simple process with a one-stage reaction was successfully realized instead of the original two-stage reaction in batch reactors. The yield of CPA reached up to 96% in only 4 min residence time at 90 °C. Interestingly, with the higher feed temperature, the reaction concentration in continuous-flow approach can be even higher than that in the batch method.
研究领域:
有机化学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）