RSC Mechanochemistry最新文献_第2页

Stainless-steel-initiated acylation of quinoxalin-2(1H)-ones with aldehydes under mechanochemical conditions† 机械化学条件下不锈钢引发的喹啉-2(1H)- 1与醛的酰化反应

RSC Mechanochemistry Pub Date : 2025-02-11 DOI: 10.1039/D4MR00131A

Diandian Wei, Zongwei Li, Heng Li and Bingxin Yuan

引用次数: 0

Chemoselectivity switch by mechanochemistry in the base-catalysed dione-acylation† 碱催化二酮酰化过程中机械化学的化学选择性开关

RSC Mechanochemistry Pub Date : 2025-02-11 DOI: 10.1039/D4MR00141A

Sally Nijem, Alexander Kaushansky, Svetlana Pucovski, Elisa Ivry, Evelina Colacino, Ivan Halasz and Charles E. Diesendruck

{"title":"Chemoselectivity switch by mechanochemistry in the base-catalysed dione-acylation†","authors":"Sally Nijem, Alexander Kaushansky, Svetlana Pucovski, Elisa Ivry, Evelina Colacino, Ivan Halasz and Charles E. Diesendruck","doi":"10.1039/D4MR00141A","DOIUrl":"https://doi.org/10.1039/D4MR00141A","url":null,"abstract":"The mechanochemistry of small molecules is an exponentially growing area of investigation relevant to developing sustainable synthesis to reduce waste and energy consumption, with great potential in large-scale chemical manufacturing. Occasionally, mechanochemical processes exhibit different reactivities, resulting in varying product selectivity compared to solution processes. In this study, we investigate the catalytic mechanism of a solvent-free one-pot acylation reaction of dimedone and 3-phenylpropanoic acid using a solvent-free ball-mill approach. The mechanochemical procedure afforded complete chemoselectivity towards a single acylation product after short milling, contrary to solution studies that previously reported product mixtures. Selectivity towards a single acylation product is controlled by the choice of the catalytic base. Under these mechanical process conditions, 4-dimethylaminopyridine (DMAP) is the only base that promotes the formation of the more desirable C-acylation product, whereas other bases exclusively afford the O-acylation product. Based on experimental findings, supported by theoretical modeling, we provide a mechanistic understanding of the base-dependent chemoselectivity, which leads to an enolate esterification that, in the case of DMAP, is converted to the thermodynamic product via Fries rearrangement. Finally, we explore the reaction scope with additional dicarbonyl compounds and carboxylic acids.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 3","pages":" 419-425"},"PeriodicalIF":0.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00141a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143913672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Green mechanochemical fabrication of graphite-lanthanide oxide nanocomposites† 石墨-氧化镧纳米复合材料的绿色机械化学制备

RSC Mechanochemistry Pub Date : 2025-02-04 DOI: 10.1039/D4MR00085D

Diego A. Acevedo-Guzmán, Brian Monroy-Torres, Petra Rudolf, Vladimir A. Basiuk and Elena V. Basiuk

{"title":"Green mechanochemical fabrication of graphite-lanthanide oxide nanocomposites†","authors":"Diego A. Acevedo-Guzmán, Brian Monroy-Torres, Petra Rudolf, Vladimir A. Basiuk and Elena V. Basiuk","doi":"10.1039/D4MR00085D","DOIUrl":"https://doi.org/10.1039/D4MR00085D","url":null,"abstract":"In this study, we explored mechanochemistry as a facile and environmentally friendly approach for the synthesis of graphite-lanthanide oxide nanocomposites. We determined the optimal conditions, namely a milling time of 48 h and milling ball size of 10 mm diameter, for which processing mixtures of graphite and lanthanide oxide in a planetary ball mill resulted in exfoliated graphene nanosheets functionalised with lanthanide oxide particles. The prepared nanocomposites were investigated by a suite of analytical techniques; X-ray photoelectron spectroscopy proved that mechanochemical processing in the presence of lanthanide oxides functionalises the graphene surface. Raman spectroscopy and X-ray diffraction results evidenced that the mechanochemical treatment exfoliates graphite and reduces the size of graphite crystallites. Scanning electron microscopy and scanning transmission electron microscopy confirmed the formation of lanthanide oxide nanoparticles and their uniform distribution on the graphene surface and thermogravimetric analysis gave evidence that the graphite-lanthanide oxide nanocomposites are less thermally stable than pristine graphite. The toxicity of the graphite-lanthanide oxide nanocomposites was also studied; we found that COS-7 monkey kidney cell growth was not inhibited for more than 5% in most of the studies.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 3","pages":" 443-458"},"PeriodicalIF":0.0,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00085d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143913675","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Reassessing mechanochemical processes in polyatomic systems for smart fabrication of nanocomposites 纳米复合材料智能制造中多原子系统机械化学过程的再评估

RSC Mechanochemistry Pub Date : 2025-01-30 DOI: 10.1039/D4MR00084F

Mamoru Senna and Adam A. L. Michalchuk

{"title":"Reassessing mechanochemical processes in polyatomic systems for smart fabrication of nanocomposites","authors":"Mamoru Senna and Adam A. L. Michalchuk","doi":"10.1039/D4MR00084F","DOIUrl":"https://doi.org/10.1039/D4MR00084F","url":null,"abstract":"A brief review is given to reassess the integrity of the fundamentals and the application in mechanochemistry. The discussion starts from the chemical response of polyatomic systems (PAS) to the mechanical stress, in terms of the extended concept of the Jahn–Teller effects. The interplay between the deformation and the chemical properties was extended to larger scale units toward solid particles or crystallites, which comprise the ensemble and arrangements of PAS. Therefore, the role of disorder of PAS arrangement or defects in solids on the reactivity of solids was discussed. Since the mechanochemical process is based on the introduction and control of the defects in solids, the discussion abridges the fundamental understanding of deformation – chemical property relationship from the basis of molecules with the reactivity of solids and powder masses. By taking the subsequent steps of relaxation in different time scales, the affordability of functional materials via a mechanochemical route has been demonstrated to finalize the entire discussion. A short summary at the end emphasises the importance of learning from the exotic fields.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 3","pages":" 351-369"},"PeriodicalIF":0.0,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00084f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143913614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Catalytic transfer hydrogenation of furfural using mechanically activated MgO as catalyst† 机械活化氧化镁催化糠醛转移加氢

RSC Mechanochemistry Pub Date : 2025-01-28 DOI: 10.1039/D4MR00128A

Antonio Manuel Pérez-Merchán, Benjamín Torres-Olea, Marcella Scala, Nikolaos Dimitratos, Irene Malpartida, Cristina García-Sancho, Josefa M. Mérida-Robles, Pedro Maireles-Torres, Ramón Moreno-Tost and Juan Antonio Cecilia

{"title":"Catalytic transfer hydrogenation of furfural using mechanically activated MgO as catalyst†","authors":"Antonio Manuel Pérez-Merchán, Benjamín Torres-Olea, Marcella Scala, Nikolaos Dimitratos, Irene Malpartida, Cristina García-Sancho, Josefa M. Mérida-Robles, Pedro Maireles-Torres, Ramón Moreno-Tost and Juan Antonio Cecilia","doi":"10.1039/D4MR00128A","DOIUrl":"https://doi.org/10.1039/D4MR00128A","url":null,"abstract":"Several MgO materials have been prepared throughout wet flow semi-continuous mechanochemical treatment of the Mg(OH)2 precursors and their subsequent calcination. This mechanochemical treatment of the precursors has shown a clear influence on the textural properties and the amount and strength of basic sites of the MgO catalysts after its calcination, obtaining higher values than that observed in a MgO sample synthesized without mechanochemical treatment. An in-depth investigation was conducted on the effects of the mechanochemical treatment on the catalytic performance in the catalytic transfer hydrogenation of furfural, and a positive effect on the activity of the catalysts was found after short mechanochemical treatment times. The highest conversion values at shorter reaction times were obtained after a mechanochemical treatment of 15 min, reaching a furfuryl alcohol yield of 79% after 2 h of reaction at 90 °C, using 2-propanol as both hydrogen donor and solvent. This data notably improves that obtained for the untreated material, which only reaches a conversion of 48% under the same experimental conditions. The stability of the material in the reaction media as well as their reusability were also investigated, and the interaction nature of 2-propanol with the MgO surface has been elucidated by attenuated total reflection spectroscopy and 2-propanol adsorption studies.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 3","pages":" 432-442"},"PeriodicalIF":0.0,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00128a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143913674","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Access to enzyme@porous organic framework biocomposites based on mechanochemical synthesis 获得enzyme@porous基于机械化学合成的有机框架生物复合材料

RSC Mechanochemistry Pub Date : 2025-01-24 DOI: 10.1039/D4MR00134F

Qing Chen, Zhi-Wei Li, Siming Huang, Guosheng Chen and Gangfeng Ouyang

{"title":"Access to enzyme@porous organic framework biocomposites based on mechanochemical synthesis","authors":"Qing Chen, Zhi-Wei Li, Siming Huang, Guosheng Chen and Gangfeng Ouyang","doi":"10.1039/D4MR00134F","DOIUrl":"https://doi.org/10.1039/D4MR00134F","url":null,"abstract":"Enzymes serve as highly efficient and selective biological catalysts, essential across diverse fields such as industry, medicine, and biotechnology, and are vital to green chemistry due to their efficacy at ambient temperatures. However, enzymes are sensitive to environmental conditions, which restricts their stability and reusability, limiting their broader practical applications. Porous organic frameworks encompassing metal–organic frameworks, covalent organic frameworks, and hydrogen-bonded organic frameworks have emerged as robust platforms for enzyme immobilization, offering high porosity, tailored pore structures, and strong chemical stability to safeguard encapsulated enzymes. Traditional surface immobilization methods can stabilize enzymes but often encounter low loading efficiency and enzyme leaching issues. In situ embedding methods address these challenges but typically rely on solvent-intensive, high-temperature liquid-phase syntheses that compromise enzyme functionality. This review centers on mechanochemical synthesis as a novel, green approach to creating enzyme-embedded porous organic frameworks, referred to as enzyme@porous organic frameworks. By employing mild mechanical forces, mechanochemical synthesis facilitates enzyme encapsulation under ambient conditions in the absence (or near-absence) of solvents, maintaining enzyme stability while ensuring efficient precursor-enzyme integration. We explore the mechanochemical synthesis principles, influential parameters, and advantages over liquid-phase techniques, underscoring its potential to produce multifunctional biocomposites. This review aspires to pave the way for scalable biocatalytic systems with enhanced stability and performance, advancing biocatalysis in industrial applications.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 3","pages":" 336-350"},"PeriodicalIF":0.0,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00134f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143913613","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemodivergent and diastereoselective synthesis of syn- and anti-cyclopentenyl spiroisoxazolones under ball-milling conditions† 球磨条件下化学发散和非对映选择性合成正、反环戊基螺异恶唑酮类化合物

RSC Mechanochemistry Pub Date : 2025-01-14 DOI: 10.1039/D4MR00125G

Peng Xu, Ming-Jun Li, Honglin Diao, Ning Shao, Zeng-Yang He, Shi-Zhu Fan, Ze Zhang and Hui Xu

引用次数: 0

Increasing the number of cations in layered double hydroxides via mechanochemically complemented synthesis: the more the merrier, or not?† 通过机械化学补充合成增加层状双氢氧化物中阳离子的数量：越多越好，还是不是？__

RSC Mechanochemistry Pub Date : 2025-01-10 DOI: 10.1039/D4MR00102H

Evgeniy Seliverstov, Maksim Yapryntsev, Evgeniya Tarasenko and Olga Lebedeva

{"title":"Increasing the number of cations in layered double hydroxides via mechanochemically complemented synthesis: the more the merrier, or not?†","authors":"Evgeniy Seliverstov, Maksim Yapryntsev, Evgeniya Tarasenko and Olga Lebedeva","doi":"10.1039/D4MR00102H","DOIUrl":"https://doi.org/10.1039/D4MR00102H","url":null,"abstract":"A series of layered double hydroxides Mg/Al, MgNi/Al, MgNi/AlIn, MgNiCo/AlIn, MgNiCo/AlInSc, and MgNiCo/AlInScTm were obtained via mechanochemically complemented synthesis with subsequent hydrothermal treatment and additional crystallization. All the samples, except for the Mg/Al one, which was similar to the meixnerite structure, were phase pure. The samples were characterized via X-ray diffraction, FTIR spectroscopy, Raman spectroscopy, and transmission electron microscopy. The peroxidase-like activity of the samples was estimated, and the crystal lattice parameters were calculated. Samples with five, six, and seven cations were characterized by X-ray fluorescence, according to which the cation ratios of the samples and the values of configurational entropy were calculated, which allowed them to be classified as high-entropy materials. For the six-cation sample, elemental mapping was additionally performed, which revealed a uniform distribution of elements over the sample area, along with high-temperature X-ray diffraction, which was also carried out for the five-cation sample.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 2","pages":" 307-316"},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00102h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143553684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Moving mechanochemistry forward 推动机械化学向前发展

RSC Mechanochemistry Pub Date : 2025-01-07 DOI: 10.1039/D4MR90021A

James Batteas, Kerstin G. Blank, Evelina Colacino, Franziska Emmerling, Tomislav Friščić, James Mack, Jeffrey Moore, Maria Elena Rivas and Wilfred Tysoe

引用次数: 0

Solvent-free zinc-mediated Béchamp reduction using mechanochemistry† 无溶剂锌介导的机械化学还原法†

RSC Mechanochemistry Pub Date : 2025-01-07 DOI: 10.1039/D4MR00138A

Koji Kubota, Asahi Nagao and Hajime Ito

引用次数: 0