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Enantioselective synthesis of (R)-citronellal from geraniol with an immobilised copper alcohol oxidase and ene reductase.
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-03 DOI: 10.1039/d5re00034c
Beatrice Tagliabue, Christian M Heckmann, Rocio Villa, Sacha Grisel, Jean-Guy Berrin, Mickael Lafond, David Ribeaucourt, Caroline E Paul

(R)-Citronellal is one of the key chiral intermediates in the synthesis of the isomer (-)-menthol, one of the most commercialised terpenoid flavours worldwide. Enzymatic approaches could represent a less energy-demanding alternative for its synthesis, such as a previously reported bienzymatic cascade starting from inexpensive, commercially available geraniol. A copper radical oxidase (CgrAlcOx) followed by a flavin-dependent ene reductase (OYE2) were used to obtain (R)-citronellal. Here, we used a metal-affinity immobilisation strategy on the His-tagged enzymes for the cascade and studied enzyme recovery and reusability as well as increased solvent tolerance. After screening a panel of resins for enzyme immobilisation and water-immiscible co-solvents, we successfully obtained 95% conversion to (R)-citronellal with 96.9% enantiomeric excess (ee) in a concurrent cascade after 7 h of reaction time, starting from 10 mM of geraniol.

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引用次数: 0
Correction: Intensification of silver nanoparticle synthesis through continuous flow split and recombine microreactors
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-30 DOI: 10.1039/D5RE90004B
Amritendu Bhuson Ghosh, Rakesh Kumar and Arnab Atta

Correction for ‘Intensification of silver nanoparticle synthesis through continuous flow split and recombine microreactors’ by Amritendu Bhuson Ghosh et al., React. Chem. Eng., 2024, 9, 1707–1720, https://doi.org/10.1039/D4RE00025K.

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引用次数: 0
Correction: Rare-earth doped hexagonal NaYbF4 nanoprobes with size-controlled and NIR-II emission for multifunctional applications 更正:用于多功能应用的稀土掺杂六方 NaYbF4 纳米探针,具有尺寸控制和 NIR-II 发射功能
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-29 DOI: 10.1039/D5RE90005K
Yu Min, Xin Ding, Bing Yu, Hailin Cong and Youqing Shen

Correction for ‘Rare-earth doped hexagonal NaYbF4 nanoprobes with size-controlled and NIR-II emission for multifunctional applications’ by Yu Min et al., React. Chem. Eng., 2023, 8, 2258–2269, https://doi.org/10.1039/D3RE00168G.

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引用次数: 0
Self-optimising continuous-flow hydrothermal reactor for nanoparticle synthesis† 用于纳米粒子合成的自优化连续流水热反应器†
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-09 DOI: 10.1039/D4RE00339J
Cameron Jackson, Karen Robertson, Vitaliy Sechenyh, Thomas W. Chamberlain, Richard A. Bourne and Edward Lester

An autonomous continuous-flow, hydrothermal synthesis reactor, capable of self-optimising nanoparticle size using an in-line characterisation technique and machine learning is presented. The developed system is used for synthesis of hematite (α-Fe2O3) nanoparticles across three process variables, optimising for a target particle size. Optimisation is achieved in under 7 h with only 500 ml of 0.1 M Fe(NO3)3·9H2O aqueous stock solution used, and without human intervention.

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引用次数: 0
Efficient and convenient synthesis of methyl (S)-5-chloro-2-hydroxy-1-oxo-2,3-dihydro-1H-indene-2-carboxylate: a key intermediate for (S)-indoxacarb using aqueous TBHP as oxidant†
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-06 DOI: 10.1039/D4RE00510D
Yun Zhang, Yao Du, Yan-Biao Chen, Jia-Huan Nie, Yue Xiong, Bao-Dong Cui, Xue-Qing Mou, Ming-Qiang Zhou and Yong-Zheng Chen

Indoxacarb is a novel broad-spectrum oxadiazine insecticide, and only (S)-indoxacarb is the active ingredient. (S)-5-Chloro-2-hydroxy-1-oxo-2,3-dihydro-1H-indene-2-carboxylate is the key intermediate for synthesising (S)-indoxacarb. However, the current process for producing the intermediate is inconvenient and difficult to scale up. Herein, we report an improved protocol for the efficient, highly stereoselective and industrially feasible preparation of the intermediate, which features the use of tert-butyl hydroperoxide (TBHP, 70% in H2O) as oxidant, purification by filtration and mild conditions.

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引用次数: 0
Interaction of light with gas-liquid interfaces: influence on photon absorption in continuous-flow photoreactors. 光与气液界面的相互作用:对连续流光反应器中光子吸收的影响。
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-06 DOI: 10.1039/d4re00540f
Jasper H A Schuurmans, Stefan D A Zondag, Arnab Chaudhuri, Miguel Claros, John van der Schaaf, Timothy Noël

Light interacts with gas bubbles in various ways, potentially leading to photon losses in gas-liquid photochemical applications. Given that light is a valuable 'reagent', understanding these losses is crucial for optimizing reactor efficiency. In this study, we address the challenge of quantifying these interactions by implementing a method that separately determines the photon flux and utilizes actinometric experiments to determine the effective optical path length, a key descriptor of photon absorption. The results reveal the unexpected impact of gas phase introduction in continuous-flow photoreactors. Notably, photon absorption, and consequently the throughput of a photoreactor, can be increased by the introduction of a gas phase. This enhancement arises from the reflection and refraction effects of gas bubbles, which can intensify light intensity in the liquid volume and thereby offset any loss in residence time. The photon absorption losses that were observed were associated with large bubbles and were less significant than anticipated. In contrast, the introduction of small bubbles was found to increase photon absorption, suggesting it is a potential strategy to optimize photoreactor performance.

光以各种方式与气泡相互作用,可能导致气液光化学应用中的光子损失。鉴于光是一种有价值的“试剂”,了解这些损失对于优化反应堆效率至关重要。在本研究中,我们通过实现一种方法来解决量化这些相互作用的挑战,该方法分别确定光子通量,并利用光光度实验来确定有效光程长度,这是光子吸收的关键描述符。结果揭示了气相引入对连续流光反应器的意外影响。值得注意的是,光子吸收,从而光反应器的吞吐量,可以通过引入气相来增加。这种增强来自气泡的反射和折射效应,它可以增强液体体积中的光强度,从而抵消任何停留时间的损失。观察到的光子吸收损失与大气泡有关,比预期的要小。相比之下,发现小气泡的引入增加了光子吸收,这表明它是优化光反应器性能的潜在策略。
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引用次数: 0
A novel core–shell bimetallic ZrAl-MOF simultaneously boosting electrostatic attraction and ion exchange to eliminate excessive fluoride†
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-23 DOI: 10.1039/D4RE00452C
Zhiwei Liu, Jingjing Wang, Qian Liu, Liying Wang, Zhenzhu Cao and Yongfeng Zhang

Excess fluoride in drinking water can cause poisoning. To solve this problem, a porous metal–organic framework (MOF) was fabricated via the solvothermal approach and employed for the removal of fluoride ions from water. ZrAl-MOF was fabricated by self-assembly of polyvalent Zr4+, Al3+metal ions and 4,4-biphenyldicarboxylic acid (BPDC). The developed metal-based ZrAl-MOF was used to remove fluoride ions from water and could remove fluoride ions to a maximum of 109.2 mg g−1 (308 K). ZrAl-MOF has a special core–shell structure with a layer of small balls stacked outside and cobweb-like structure inside. The properties of the bimetallic MOF can be adjusted by Zr4+, Al3+ metal ions and BPDC to meet the demand for maximum adsorption performance. Bimetallic MOFs commonly have a substantial specific surface area, capable of providing numerous active sites and being favorable for the adsorption reaction of substances. The electronic properties of different metals may lead to stronger electrostatic attraction and enhanced adsorption of fluoride ions. The factors affecting the adsorption effect, such as solution pH, ZrAl-MOF dosage, reaction time, initial fluoride concentration, temperature, and coexisting anions, were optimized. The fluorine adsorption capacity of ZrAl-MOF was less affected by the adsorbent under acidic conditions and by the presence of sulphate and nitrate ions in the water. In addition, the experimental data were fitted with various adsorption kinetic and isotherm models. It is shown that fluorine adsorption is feasible and spontaneous. The fluorine adsorption mechanism of ZrAl-MOF is mainly electrostatic attraction and ion exchange.

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引用次数: 0
Structured internals for the intensified Fischer–Tropsch synthesis in fixed-bed reactors†
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-23 DOI: 10.1039/D4RE00550C
Evert Boymans, Yadolah Ganjkhanlou, Marco Denneman, Ben Sutens, Jasper Lefevere and Sander Grootjes

To accelerate the energy transition, processes for the production of sustainable fuels are desired such as the conversion of syngas from biogenic residues into liquid fuel by using the Fischer–Tropsch synthesis (FTS). These novel conversion processes are often of smaller scale due to the feedstock for which intensified reactor concepts are required. Structured reactors present viable alternatives to conventional packed bed reactors. Structured reactors can be obtained by e.g. loading a conventional tubular reactor with structured internals. Here, two strategies were followed in an effort to obtain the highest productivity per reactor volume, namely application of 3D-printed catalysts and secondly, thermally conductive aluminium and copper contactors filled with catalyst particles. Superior productivities were obtained by applying Al foam and 3D-printed Cu contactors when packed with FTS catalyst particles, with heat duties of respectively 880 kW m−3 and 1238 kW m−3 compared with only 185 kW m−3 for the 3D-printed catalyst and 218 kW m−3 for a conventional packed bed. For the system using the ordered 3D-printed Cu contactors, it presented a productivity of at least 0.85 gC5+ gcat−1 h−1. The excellent productivities could be correlated to the high thermal conductivity of the metal contactors facilitating the heat transfer from the bed centreline to the reactor wall as revealed by laser flash analysis (LFA) thermal conductivity measurements.

为加快能源转型,人们希望采用生产可持续燃料的工艺,如利用费托合成(FTS)将生物残留物中的合成气转化为液体燃料。由于原料的原因,这些新型转化工艺通常规模较小,因此需要强化的反应器概念。结构化反应器是传统填料床反应器的可行替代品。结构化反应器可以通过在传统管式反应器上加载结构化内件等方式获得。为了获得最高的单位反应器容积生产率,我们采用了两种策略,一是应用 3D 打印催化剂,二是在导热铝和铜接触器中填充催化剂颗粒。在使用泡沫铝和三维打印铜接触器填充 FTS 催化剂颗粒时,可获得更高的生产率,热负荷分别为 880 kW m-3 和 1238 kW m-3,而三维打印催化剂的热负荷仅为 185 kW m-3,传统填料床的热负荷为 218 kW m-3。对于使用有序三维打印铜接触器的系统,其生产率至少为 0.85 gC5+ gcat-1 h-1。激光闪烁分析(LFA)热导率测量结果表明,出色的生产率与金属接触器的高热导率有关,它促进了从床层中心线到反应器壁的热传导。
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引用次数: 0
The road to green efficiency: exploration of multicomponent reactions from transition metal catalysis to no catalyst conditions 绿色效率之路:从过渡金属催化到无催化剂条件下的多组分反应探索
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-20 DOI: 10.1039/D4RE00522H
Jie Li, Jiajun Cui, Hongying Guo, Jiyou Yang and Weiwei Huan

During the past decade, multicomponent reactions (or MCRs) have become excellent tools for rapidly synthesizing structurally complex and high-value small molecules. In particular, the development of MCRs for building molecules of interest in biology and medicine has been receiving increasing attention due to their simplicity, efficiency, and convergent advantages. They have widespread applications in drug development, materials science, and biomedicine. It is noteworthy that MCRs typically have features such as mild conditions and universal compatibility with green solvents, highlighting their green sustainability. This minireview highlights recent progress in MCRs under different catalytic conditions until 2024. We classify the content of the review according to the type of catalyst in order to offer a better overview and deeper understanding to the readership, hoping this work will exhibit the charm of multicomponent reactions.

在过去十年中,多组分反应(MCR)已成为快速合成结构复杂和高价值小分子的绝佳工具。特别是,由于多组分反应具有简便、高效和会聚的优势,开发多组分反应来构建生物学和医学领域感兴趣的分子已受到越来越多的关注。它们在药物开发、材料科学和生物医学领域有着广泛的应用。值得注意的是,MCR 通常具有条件温和、与绿色溶剂普遍兼容等特点,突出了其绿色可持续性。本微型综述重点介绍了 2024 年前不同催化条件下 MCR 的最新进展。我们根据催化剂的类型对综述内容进行了分类,以便读者更好地了解和深入理解,希望这些工作能展现多组分反应的魅力。
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引用次数: 0
Correction: Combination of near-infrared spectroscopy and a transient flow method for efficient kinetic analysis of the Claisen rearrangement
IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-19 DOI: 10.1039/D4RE90043J
Yoshihiro Takebayashi, Kiwamu Sue and Sho Kataoka

Correction for ‘Combination of near-infrared spectroscopy and a transient flow method for efficient kinetic analysis of the Claisen rearrangement’ by Yoshihiro Takebayashi et al., React. Chem. Eng., 2024, 9, 2975–2983, https://doi.org/10.1039/D4RE00301B.

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引用次数: 0
期刊
Reaction Chemistry & Engineering
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