Reaction Chemistry & Engineering最新文献

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High CO conversion in syngas to aromatics by addition of ZnMnZr oxides as methanol synthesis components† 添加ZnMnZr氧化物作为甲醇合成组分,可提高合成气中CO的芳烃转化率
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-21 DOI: 10.1039/D5RE00078E
Shiyu Liu, Qiuyun Huang, Jie Wang, Weihua Shen and Yunjin Fang
{"title":"High CO conversion in syngas to aromatics by addition of ZnMnZr oxides as methanol synthesis components†","authors":"Shiyu Liu, Qiuyun Huang, Jie Wang, Weihua Shen and Yunjin Fang","doi":"10.1039/D5RE00078E","DOIUrl":"https://doi.org/10.1039/D5RE00078E","url":null,"abstract":"<p >In the oxide-zeolite (OX-ZEO) strategy, it is challenging to achieve both higher CO conversion and aromatics selectivity. In this paper, the methanol synthesis component <em>x</em>Zn2Mn8Zr was prepared. With increasing Zn content, CO conversion over the ternary oxides increased without a remarkable decrease in the combined selectivity of methanol and dimethyl ester (DME). The 2Zn2Mn8Zr (molar ratio) was then coupled with either SAPO-34 or H-ZSM-5 for syngas conversion. Combined with the results of thermogravimetric analysis, a bifunctional catalyst with more residual hydrocarbon pool species (HCPs) was capable of achieving higher selectivity of unsaturated organic products. The loss of HCPs should be attributed to over-hydrogenation. The over-hydrogenation could be related to either Zn concentration or the close contact of 2Zn2Mn8Zr with H-ZSM-5. To alleviate such over-hydrogenation, ZnMnZr pellets with lower Zn concentration were mixed with the pellets of 6Mn4Zr/H-ZSM-5 using a granule mixing method. The multi-functional catalyst exhibited much higher activity in syngas-to-aromatics (STA) conversion, especially at high space velocities. The CO conversion over the multi-functional catalyst could reach 43% at 600 mL g<small><sub>cat</sub></small><small><sup>−1</sup></small> h<small><sup>−1</sup></small>, with aromatics selectivity around 72%, and it remained stable during a 100 h reaction.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 8","pages":" 1803-1811"},"PeriodicalIF":3.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144680945","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Kinetic and mechanistic studies of cyclohexane oxidation with tert-butyl hydroperoxide over M–N4 catalysts† M-N4催化剂催化过氧化叔丁基氧化环己烷的动力学和机理研究
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-21 DOI: 10.1039/D5RE00031A
Ethan P. Iaia, Miles G. Miller, Ademola Soyemi, Martin G. Bakker, Tibor Szilvási and James W. Harris
{"title":"Kinetic and mechanistic studies of cyclohexane oxidation with tert-butyl hydroperoxide over M–N4 catalysts†","authors":"Ethan P. Iaia, Miles G. Miller, Ademola Soyemi, Martin G. Bakker, Tibor Szilvási and James W. Harris","doi":"10.1039/D5RE00031A","DOIUrl":"https://doi.org/10.1039/D5RE00031A","url":null,"abstract":"<p >Oxidation of cyclohexane with <em>tert</em>-butyl hydroperoxide (TBHP) is a common probe reaction for molecular complexes, though the kinetics of this reaction are seldom reported. Here, we synthesize metal–nitrogen-doped carbons (M-N-Cs) and a series of zeolite-encapsulated metal phthalocyanine (MPC) catalysts and compare their reactivity in cyclohexane oxidation with TBHP. These materials all have primary binding sites that include square planar metals bound to four nitrogen atoms (M–N<small><sub>4</sub></small> sites). We measure the apparent activation energy for this reaction, and compare the reactivity of M-N-C and MPC catalysts with varied metal central atoms (M = Fe, Mn, Co, Cu, Cr, Ni), of which Fe-containing catalysts are the most reactive. Fe-N-C catalysts are more stable with reuse than FePC catalysts. Apparent reaction orders are less than one for both reactants, suggesting a surface mediated reaction. Cyclohexanol and cyclohexanone form in parallel at short reaction times, while cyclohexanol further reacts to cyclohexanone at longer reaction times. DFT calculations show that the reaction may follow a radical-mediated Eley–Rideal mechanism that is primarily mediated <em>via tert</em>-butoxy radicals formed at the metal site. Microkinetic modeling of the proposed mechanism reproduces experimental trends in product rates and selectivity of the main reaction products without requiring any parameter estimation. This study demonstrates that M-N-C and MPC catalysts perform cyclohexane oxidation with TBHP with similar per metal-atom initial rates. These results will enable judicious use of cyclohexane oxidation with TBHP as a probe reaction to compare reactivity of catalysts with M–N<small><sub>4</sub></small> active sites.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1647-1664"},"PeriodicalIF":3.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472769","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A waste-free packed-bed continuous-flow synthesis of disulfiram with a composite catalyst† 用复合催化剂制备无废填料床连续流法合成双硫仑
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-18 DOI: 10.1039/D5RE00028A
Yu-Zhen Xue, Xing-Jian Li, Ze-Run Zhao, Hao-Xing Xu, Shun-Guo Fu, Fang-Xiao Wang and Xiao Wang
{"title":"A waste-free packed-bed continuous-flow synthesis of disulfiram with a composite catalyst†","authors":"Yu-Zhen Xue, Xing-Jian Li, Ze-Run Zhao, Hao-Xing Xu, Shun-Guo Fu, Fang-Xiao Wang and Xiao Wang","doi":"10.1039/D5RE00028A","DOIUrl":"https://doi.org/10.1039/D5RE00028A","url":null,"abstract":"<p >Disulfiram, a star molecule in the rubber, pharmaceutical and agrochemical industries, has been encountering multiple challenges for its conventional synthesis. In this work, a highly sustainable and efficient MoS<small><sub>2</sub></small>-catalyzed continuous-flow synthesis of TETD has been developed, providing high yield and purity of products upon simple isolation. This process uses O<small><sub>2</sub></small> and ethanol as a green oxidant and solvent, without any sacrificing redox agent, rendering it fully atom-economic. The packed-bed filled with MoS<small><sub>2</sub></small> and the co-catalyst Ca(OH)<small><sub>2</sub></small> is low-leaching and reusable. The structurally similar rubber accelerator tetramethylthiuram disulfide (TMTD) was also synthesized using this method.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 8","pages":" 1795-1802"},"PeriodicalIF":3.4,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144680944","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Reactor intensification on glycerol-to-acrylic acid conversion: a modelling study† 反应器强化对甘油到丙烯酸的转化:一个模型研究†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-16 DOI: 10.1039/D4RE00481G
Prashant Pawanipagar, Kamran Ghasemzadeh, Carmine D'Agostino and Vincenzo Spallina
{"title":"Reactor intensification on glycerol-to-acrylic acid conversion: a modelling study†","authors":"Prashant Pawanipagar, Kamran Ghasemzadeh, Carmine D'Agostino and Vincenzo Spallina","doi":"10.1039/D4RE00481G","DOIUrl":"https://doi.org/10.1039/D4RE00481G","url":null,"abstract":"<p >This work presents a numerical analysis for glycerol dehydration &amp; acrolein oxidation to produce acrylic acid and determine the optimal process conditions combining computational fluid dynamics (CFD) with response surface methodology (RSM) techniques. For glycerol dehydration, optimum conditions are found at 623 K, 5731.6 h<small><sup>−1</sup></small> GHSV, and a glycerol mass fraction of 0.32, resulting in a glycerol conversion of 94.2% and an acrolein selectivity of 79.6%. Further, the simulations with optimized conditions for two proposed configurations have insignificant glycerol conversion and acrolein selectivity suggesting that alternative reactor configurations have limited improvement. In the case of the acrolein selective oxidation process, an optimum temperature of 583.5 K, a GHSV of 1600 h<small><sup>−1</sup></small>, and an oxygen-to-acrolein molar ratio of 5.73 result in an acrylic acid yield and a selectivity of 80.9% and 87.5%, respectively. In the case of a membrane reactor with distributed oxygen feeding, the acrylic acid yield reached 85.9% and it exhibits a remarkable selectivity of 97.1%.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 8","pages":" 1812-1827"},"PeriodicalIF":3.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d4re00481g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144680946","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
New dispersible and low-melting cellulose ester produced with molten adipic acid as a solvent, reagent and catalyst, and its application to improve the mechanical properties of PLA† 以熔融己二酸为溶剂、试剂和催化剂制备新型分散性低熔点纤维素酯,及其在改善PLA†力学性能中的应用
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-16 DOI: 10.1039/D5RE00080G
Mariafrancesca Baratta, Fabrizio Olivito, Cataldo Simari, Wan Abd Al Qadr Imad Wan-Mohtar, Isabella Nicotera, Fiore Pasquale Nicoletta, Giovanni De Filpo and Giovanni Golemme
{"title":"New dispersible and low-melting cellulose ester produced with molten adipic acid as a solvent, reagent and catalyst, and its application to improve the mechanical properties of PLA†","authors":"Mariafrancesca Baratta, Fabrizio Olivito, Cataldo Simari, Wan Abd Al Qadr Imad Wan-Mohtar, Isabella Nicotera, Fiore Pasquale Nicoletta, Giovanni De Filpo and Giovanni Golemme","doi":"10.1039/D5RE00080G","DOIUrl":"https://doi.org/10.1039/D5RE00080G","url":null,"abstract":"<p >The synthesis of a new cellulose ester (CE) from microcrystalline cellulose (MCC) and adipic acid is described. The solvent-free reaction was carried at 155 °C, slightly above the melting point of adipic acid. The molten acid is both the reactant and the Brønsted acid catalyst in this reaction. Cellulose adipate is highly crystalline and the modification of the XRD powder pattern with respect to MCC indicates that the spatial arrangement of the pristine cellulose Iβ and its hydrogen bonding network have drastically changed. According to TGA and XRD, esterified cellulose surrounds a core of intact MCC (25% by weight), however, the new cellulose adipate material has a melting point of 153 °C and is dispersable in chlorinated solvents. The composites with PLA were prepared by the solvent casting method. The best results were obtained using 3 wt% of the cellulose ester, with a maximum elongation increased by 59%, and a reduction of the tensile strength of 25% only. The SEM images of the best PLA composite show the absence of the cracks found in the PLA films. This work demonstrates how value-added materials can be prepared from renewable and readily available resources through green and sustainable technologies.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1615-1626"},"PeriodicalIF":3.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d5re00080g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472766","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A PLC based semi-automated extraction chromatographic separation system for the isolation of medical grade no-carrier-added lutetium-177 for targeted cancer therapy† 一种基于PLC的半自动化萃取色谱分离系统,用于分离用于靶向癌症治疗的医用级无载体添加的镥-177
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-14 DOI: 10.1039/D4RE00574K
Dheeraj Kumar, Aaditya Shah, Varun Nair, B. K. Tiwary, N. C. Joseph, Abhishek K. Sharma, Arpit Mitra, Navin Sakhare, Sanjeev Kumar, Chanda Arjun, K. V. V. Nair, Anupam Mathur, Sudipta Chakraborty, Usha Pandey, Ameya Puranik, Archi Agrawal and Venkatesh Rangarajan
{"title":"A PLC based semi-automated extraction chromatographic separation system for the isolation of medical grade no-carrier-added lutetium-177 for targeted cancer therapy†","authors":"Dheeraj Kumar, Aaditya Shah, Varun Nair, B. K. Tiwary, N. C. Joseph, Abhishek K. Sharma, Arpit Mitra, Navin Sakhare, Sanjeev Kumar, Chanda Arjun, K. V. V. Nair, Anupam Mathur, Sudipta Chakraborty, Usha Pandey, Ameya Puranik, Archi Agrawal and Venkatesh Rangarajan","doi":"10.1039/D4RE00574K","DOIUrl":"https://doi.org/10.1039/D4RE00574K","url":null,"abstract":"&lt;p &gt;Extensive clinical deployment of lutetium-177 (&lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu) radiopharmaceuticals for targeted cancer therapy has led to an increased demand of &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu-radionuclides all over the world. Since most of the clinically established targeted cancer therapies involve receptor targeting peptides, enzyme inhibitors or antibodies, the use of high specific activity &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu is necessary to prepare &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu complexes in high molar activity to obtain maximum efficacy of treatment. Therefore, there is an immense interest in the production of clinical grade no carrier added (NCA) &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu globally. While carrier added &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu can be produced by the neutron activation of an enriched &lt;small&gt;&lt;sup&gt;176&lt;/sup&gt;&lt;/small&gt;Lu target, NCA&lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu is produced by neutron activation of an enriched &lt;small&gt;&lt;sup&gt;176&lt;/sup&gt;&lt;/small&gt;Yb target &lt;em&gt;via&lt;/em&gt; the &lt;small&gt;&lt;sup&gt;176&lt;/sup&gt;&lt;/small&gt;Yb (n, γβ) &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu reaction. The present work describes a semi-automated extraction chromatography-based modular separation system, which can be conveniently adopted for rapid isolation of medical grade NCA &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu from the neutron irradiated enriched &lt;small&gt;&lt;sup&gt;176&lt;/sup&gt;&lt;/small&gt;Yb target. The separation module is based on multistage extraction chromatography using LN2 and DGA resins (3 stage each). Herein, we demonstrate effective utilization of this system to separate &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu from the irradiated enriched &lt;small&gt;&lt;sup&gt;176&lt;/sup&gt;&lt;/small&gt;Yb target (+96.4%, 50–150 mg). The process could be completed within a short period of 4–5 h with overall 70–74% (26.6–74.0 GBq) &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu recovery. The HPGe and ICP-AES analysis results for a typical batch indicated Yb impurity below 0.1% in isolated &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu. The &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu specific activity obtained was ∼1.6 GBq mg&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; of lutetium. The NCA &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;LuCl&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt; obtained by this route qualified all the necessary quality control tests for human use. To demonstrate the clinical utility, the NCA &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;LuCl&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt; activity was used for the preparation of patient doses each of &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu-DOTA-TATE (7.4 GBq) and &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu-PSMA-617 (7.4 GBq). The 24 h post-therapy SPECT scan of the two cancer patients injected with the respective &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;Lu-radiopharmaceuticals (5.5–7.4 GBq) were in concordance with the corresponding &lt;small&gt;&lt;sup&gt;68&lt;/sup&gt;&lt;/small&gt;Ga-PET scans. The PLC based semi-automated separation system reported herein demonstrates the feasibility of NCA &lt;small&gt;&lt;sup&gt;177&lt;/sup&gt;&lt;/small&gt;LuCl&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt; production in a short span of time, which can be effectively implemented at the commercial scale fo","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1569-1576"},"PeriodicalIF":3.4,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Proton exchange membrane flow reactor with ozone-treated gas diffusion layers for production of pure H2O2 in aqueous and methanol solutions† 质子交换膜流动反应器与臭氧处理的气体扩散层生产纯H2O2在水和甲醇溶液†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-12 DOI: 10.1039/D4RE00634H
Takuya Okazaki, Chihiro Tateishi, Kento Shibata, Kazuma Enomoto and Fumiaki Amano
{"title":"Proton exchange membrane flow reactor with ozone-treated gas diffusion layers for production of pure H2O2 in aqueous and methanol solutions†","authors":"Takuya Okazaki, Chihiro Tateishi, Kento Shibata, Kazuma Enomoto and Fumiaki Amano","doi":"10.1039/D4RE00634H","DOIUrl":"https://doi.org/10.1039/D4RE00634H","url":null,"abstract":"<p >Electrocatalytic production of pure H<small><sub>2</sub></small>O<small><sub>2</sub></small><em>via</em> the two-electron oxygen reduction reaction (2e<small><sup>−</sup></small> ORR) in a proton exchange membrane (PEM) flow reactor is an ideal process for on-site and on-demand H<small><sub>2</sub></small>O<small><sub>2</sub></small> usage. However, the low selectivity is challenging due to the successive reduction of generated H<small><sub>2</sub></small>O<small><sub>2</sub></small> remaining on the electrocatalyst in a membrane electrode assembly with a gas diffusion layer (GDL). This study investigates the selective 2e<small><sup>−</sup></small> ORR in an H<small><sub>2</sub></small>–O<small><sub>2</sub></small> PEM flow reactor (PEMFR) using a cobalt electrocatalyst with various cathode GDLs to optimize the transport of solvent to recover the generated H<small><sub>2</sub></small>O<small><sub>2</sub></small>. The effects of wettability and hydrophobicity were tested using pristine, polytetrafluoroethylene (PTFE) treated, and ozone-treated carbon GDLs under simultaneous water and O<small><sub>2</sub></small> gas flow. The ozone-treated GDL, with slight hydrophilicity, continuously produced 46 mM H<small><sub>2</sub></small>O<small><sub>2</sub></small> (1560 ppm) with a faradaic efficiency (FE) of ∼75% at a current density of 20–30 mA cm<small><sup>−2</sup></small>. In contrast, pristine and PTFE-treated GDLs resulted in a low H<small><sub>2</sub></small>O<small><sub>2</sub></small> FE below 15%. The ozone-treated GDL on the flow channel side was critical for transporting liquid water to recover the generated H<small><sub>2</sub></small>O<small><sub>2</sub></small>. The production of H<small><sub>2</sub></small>O<small><sub>2</sub></small> in methanol instead of water also achieved ∼80% FE, without applying energy bias.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1638-1646"},"PeriodicalIF":3.4,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hydrogenation of nitriles to primary amines with a carbon-coated Ni/NiO@C catalyst under friendly conditions† 友好条件下碳包覆Ni/NiO@C催化剂催化腈加氢制伯胺†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-11 DOI: 10.1039/D5RE00096C
Weidong Liu and Jianguo Liu
{"title":"Hydrogenation of nitriles to primary amines with a carbon-coated Ni/NiO@C catalyst under friendly conditions†","authors":"Weidong Liu and Jianguo Liu","doi":"10.1039/D5RE00096C","DOIUrl":"https://doi.org/10.1039/D5RE00096C","url":null,"abstract":"<p >Reusable catalysts based on non-noble metals with broad applicability for nitrile catalytic hydrogenation are key to achieving more sustainable primary amine production. Herein, a simple and efficient carbon-coated non-noble nickel-based catalyst (Ni/NiO@C-600-200-1-H<small><sub>2</sub></small>O) was developed for the hydrogenation of aromatic substituted nitriles to aromatic substituted amines under relatively mild conditions (120 °C, 10 bar H<small><sub>2</sub></small>, 4 h). The carbon-coated structure endows the catalyst with excellent anti-agglomeration properties, significantly enhancing its cycling stability. The catalyst exhibits high tolerance toward various functional groups, including halogen, methyl, and methoxy, achieving remarkable conversion rates (over 99%) and product selectivity (up to 98.25%). Additionally, the catalyst's magnetic properties facilitate easy recovery and reuse. When applied to a continuous flow reactor for benzonitrile hydrogenation under optimized conditions, the catalyst demonstrated a conversion rate and selectivity exceeding 99%, with continuous operation lasting up to 31 h.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1627-1637"},"PeriodicalIF":3.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synthesis of nitrile-containing reactive phenolphthalein polyaryletherketone and synergistic toughening research on the toughening of epoxy resin—phase structure, mechanical and thermal properties 含腈反应性酚酞聚芳醚酮的合成及增强型增韧环氧树脂的相结构、力学性能和热性能研究
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-10 DOI: 10.1039/D5RE00084J
Jiawei Liu, Tongjia Zhang, Shoutian Qiu, Lixin Song, Guangyuan Zhou and Honghua Wang
{"title":"Synthesis of nitrile-containing reactive phenolphthalein polyaryletherketone and synergistic toughening research on the toughening of epoxy resin—phase structure, mechanical and thermal properties","authors":"Jiawei Liu, Tongjia Zhang, Shoutian Qiu, Lixin Song, Guangyuan Zhou and Honghua Wang","doi":"10.1039/D5RE00084J","DOIUrl":"https://doi.org/10.1039/D5RE00084J","url":null,"abstract":"<p >The introduction of reactive groups capable of participating in epoxy cross-linking into the molecular chains of conventional thermoplastic toughening agents effectively enhances the interfacial compatibility between thermoplastic and thermosetting resins, resulting in a significant improvement in system impact toughness. Building on this approach, this study innovatively incorporates polar nitrile groups into the molecular chains of thermoplastic polyaryletherketone agents containing terminal reactive groups, thereby exploring the synergistic mechanism between reactive and nitrile groups. A systematic investigation is conducted to examine how variations in the nitrile group content and the addition level of the toughening agent influence the toughening effect of epoxy resin. Additionally, the influence of different epoxy system phase structures on mechanical properties is assessed. Experimental results reveal that when the toughening agent PEKCN-OH is added at less than 10 parts per hundred resin (phr), the epoxy system exhibits a sea-island morphology, with the impact strength decreasing with increasing nitrile group content. When no nitrile groups are present (using PEKC-OH resin), the impact strength reaches 23.5 kJ m<small><sup>−2</sup></small>, representing a 97% increase compared to the control without the toughening agent. For addition levels exceeding 10 phr, the system transitions to a bicontinuous structure. In this regime, the impact strength initially increases before decreasing as the nitrile group content increases. At a nitrile group content of 50% (using PEKCN-OH-2 resin), the impact strength reaches 25.8 kJ m<small><sup>−2</sup></small>, representing a 117% increase. Importantly, the addition of these toughening agents not only prevents a reduction in the service temperature of the epoxy resin but also enhances its thermal stability. In conclusion, the PEKCN-OH developed in this study serves as a highly efficient, easily prepared reactive thermoplastic toughening agent suitable for industrial production. It holds great promise for use in demanding industrial applications, including aerospace, electronics and electrical appliances, and automotive manufacturing. The findings are expected to make significant contributions to material innovation and product performance optimization in these sectors.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1539-1550"},"PeriodicalIF":3.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Simultaneous enzymatic esterification and ester extraction in Pickering emulsions for the recovery of butanol from fermentation broth† 皮克林乳剂中同时酶促酯化和酯萃取法回收发酵液中丁醇的研究
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2025-04-10 DOI: 10.1039/D4RE00625A
Yaoyao Feng, Pierre-Louis Carrette, Christine Dalmazzone and Etienne Jourdier
{"title":"Simultaneous enzymatic esterification and ester extraction in Pickering emulsions for the recovery of butanol from fermentation broth†","authors":"Yaoyao Feng, Pierre-Louis Carrette, Christine Dalmazzone and Etienne Jourdier","doi":"10.1039/D4RE00625A","DOIUrl":"https://doi.org/10.1039/D4RE00625A","url":null,"abstract":"<p >The recovery of biobutanol from highly diluted aqueous fermentation broth usually suffers from intensive energy consumption. In this study, we developed a Pickering emulsion system stabilized by silica nanoparticles for the rapid and efficient recovery of low concentrations of butanol (&lt;20 g L<small><sup>−1</sup></small>) from fermentation broth in the form of esters. Each droplet in the emulsion system serves as a microreactor for enzymatic esterification of butanol in the water phase, and the ester product is spontaneously extracted to the oil phase, thereby promoting the esterification reaction. The system offers a significantly larger interfacial area and a 2–5 times improvement in reaction rate compared to the biphasic system. Under optimal conditions, the conversion and extraction of butanol from the fermentation broth into butyl butyrate achieved a yield of 79% in the presence of a Pickering emulsion. This study presents a sustainable and efficient approach for the recovery of biobased butanol.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 7","pages":" 1606-1614"},"PeriodicalIF":3.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d4re00625a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472765","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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