RSC Mechanochemistry最新文献_第9页

How external forces affect the degradation properties of perfluorooctanoic acid in mechanochemical degradation: a DFT study† 机械化学降解中，外力如何影响全氟辛酸的降解特性：一项DFT研究†

RSC Mechanochemistry Pub Date : 2025-06-11 DOI: 10.1039/D5MR00048C

Chuan Wang, Cheng Yang, Jie Wu, Ziqiu Wang and Kun Yang

{"title":"How external forces affect the degradation properties of perfluorooctanoic acid in mechanochemical degradation: a DFT study†","authors":"Chuan Wang, Cheng Yang, Jie Wu, Ziqiu Wang and Kun Yang","doi":"10.1039/D5MR00048C","DOIUrl":"https://doi.org/10.1039/D5MR00048C","url":null,"abstract":"Perfluorooctanoic acid (PFOA), recognized as a persistent organic pollutant, poses a serious threat to the environment and human health. Currently, mechanochemical degradation is considered a highly promising technology for the degradation of PFOA. This study systematically employs density functional theory (DFT) and the COGEF (COnstrained GEometry to simulate Forces) model to deeply investigate the impact of external forces on the degradation properties of PFOA molecules. Through quantum chemical calculations, we analyzed in detail the changes in the electronic structure, chemical reactivity, and decarboxylation reaction process of PFOA molecules under the influence of external forces. The results show that the application of external forces significantly alters the electronic density distribution of PFOA molecules, thereby enhancing their reactive activity, especially in terms of nucleophilicity and radical reactivity at the carboxylate end. Moreover, the application of external mechanical force reduces the Gibbs free energy change of the decarboxylation reaction, thereby making the reaction energetically favorable. This study not only theoretically elucidates the mechanism of mechanochemical degradation of PFOA, but also provides a basis for optimizing its mechanochemical degradation technology. In addition, this study also provides a systematic theoretical perspective for exploring the mechanisms of mechanochemical degradation.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 692-705"},"PeriodicalIF":0.0,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d5mr00048c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144929126","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

Amorphous quininium aspirinate from neat mechanochemistry: diffracting nanocrystalline domains and quick recrystallization upon exposure to solvent vapours†‡ 非晶态阿斯匹林醌从整齐的机械化学：衍射纳米晶域和快速再结晶暴露于溶剂蒸汽†‡

RSC Mechanochemistry Pub Date : 2025-06-10 DOI: 10.1039/D5MR00028A

Silvina Pagola, James Howard, Johannes Merkelbach and Danny Stam

{"title":"Amorphous quininium aspirinate from neat mechanochemistry: diffracting nanocrystalline domains and quick recrystallization upon exposure to solvent vapours†‡","authors":"Silvina Pagola, James Howard, Johannes Merkelbach and Danny Stam","doi":"10.1039/D5MR00028A","DOIUrl":"https://doi.org/10.1039/D5MR00028A","url":null,"abstract":"Quininium aspirinate is mechanochemically prepared as a crystalline solid by liquid-assisted grinding, or as an amorphous phase (as determined by X-ray powder diffraction), by neat grinding or neat ball milling. Our previous work demonstrated using FT-IR spectroscopy that a mechanochemical reaction had occurred in the mechanically treated neat mixtures. Herein is reported that microcrystal electron diffraction (microED) afforded the discovery of two diffracting micron-size particles in the amorphous powder synthesized by manual grinding, among a majority of non-diffracting particles. Remarkably, microED data of one of them led to the known lattice parameters of quininium aspirinate. Furthermore, this so-called ‘X-ray amorphous’ phase quickly recrystallizes upon exposure to vapors of N,N-dimethylformamide, or hexane vapours (at a lower rate); but it remains amorphous for longer than 20 months when stored at ambient conditions in a closed container. The lattice parameters and the degrees of crystallinity of both recrystallized materials are identical within the experimental error. However, slightly more intense and better-resolved X-ray powder diffraction peaks are observed in the material recrystallized from N,N-dimethylformamide vapours than in the analogous phase recovered from hexane. As expected, Williamson–Hall graphs lead to a larger average crystalline domain size for the former solid. These results illustrate the use of microED for the investigation of structural features in amorphous phases, and the generic role of the solvent vapours in promoting their recrystallization.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 670-679"},"PeriodicalIF":0.0,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d5mr00028a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144929143","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

Dry-vortex grinding facilitates a [2 + 2] cycloaddition reaction that triggers a cascade-like reaction that improves the yield under substoichiometric conditions† 干涡研磨促进了[2 + 2]环加成反应，引发了类似级联的反应，在亚化学计量条件下提高了产率

RSC Mechanochemistry Pub Date : 2025-06-05 DOI: 10.1039/D5MR00025D

Angela A. Colmanet, Daniel K. Unruh and Ryan H. Groeneman

引用次数: 0

Mechanochemistry assisted aqueous two-phase extraction: an efficient technique to extract high-purity juglone from the bark of Juglans mandshurica 机械化学辅助双水相萃取：从水杨树树皮中提取高纯度核桃胶酮的高效工艺

RSC Mechanochemistry Pub Date : 2025-06-03 DOI: 10.1039/D4MR00132J

Shuang Wei, Xinbiao Zhou and Jun Xi

{"title":"Mechanochemistry assisted aqueous two-phase extraction: an efficient technique to extract high-purity juglone from the bark of Juglans mandshurica","authors":"Shuang Wei, Xinbiao Zhou and Jun Xi","doi":"10.1039/D4MR00132J","DOIUrl":"https://doi.org/10.1039/D4MR00132J","url":null,"abstract":"The bark of Juglans mandshurica (BJM) is a Chinese herbal medicine containing a variety of nutrients and pharmacologically active compounds. Juglone, one of the important active ingredients in BJM, has been shown by many pharmacological studies to have antioxidant, antibacterial, antiviral, anti-tumor, immunoregulatory and other pharmacological properties. Mechanochemistry assisted aqueous two-phase extraction (MAATPE) was successfully established to extract juglone from BJM, combining the purification effect of an alcohol/salt aqueous two-phase system (ATPS) with the high efficiency of mechanochemistry. The key parameters of MAATPE were systematically optimized through single factor analysis and response surface methodology. Under the optimal conditions of an ethanol/NaH2PO4 aqueous two-phase system as the liquid reagent, 21.5% (w/w) ethanol concentration, 28% (w/w) NaH2PO4 concentration, 458 rpm milling speed, 14 min milling time and 59 mL g−1 reagent–material ratio, the maximum yield of juglone was 15.36 ± 0.16 mg g−1 with a purity of 9.82 ± 0.12% in dry extracts. Compared with other extraction methods, it was found that MAATPE can not only improve the extraction efficiency of juglone, but also achieve higher juglone purity in the products. Finally, the mechanism of action, recyclability and industrial scalability of MAATPE are discussed. In conclusion, MAATPE is an appropriate alternative for the efficient preparation of high-purity products from natural resources.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 680-691"},"PeriodicalIF":0.0,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00132j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144929141","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

Fluorination of mechanochemically synthesized metal–organic frameworks for PFAS adsorption in water† 机械化学合成金属-有机骨架在水中吸附PFAS的氟化研究

RSC Mechanochemistry Pub Date : 2025-05-27 DOI: 10.1039/D5MR00043B

Danilo Marchetti, Enrico Dalcanale, Roberta Pinalli, Mauro Gemmi, Alessandro Pedrini and Chiara Massera

引用次数: 0

Thermodynamic and kinetic study of the effect of LiCl and NaCl on the thermal dehydrogenation of Ca(AlH4)2† LiCl和NaCl对Ca(AlH4)2†热脱氢影响的热力学和动力学研究

RSC Mechanochemistry Pub Date : 2025-05-13 DOI: 10.1039/D4MR00140K

Franziska Habermann, Anneliese Wirth, Konrad Burkmann, Jakob Kraus, Bianca Störr, Hartmut Stöcker, Jürgen Seidel, Jens Kortus, Roman Gumeniuk, Klaus Bohmhammel and Florian Mertens

引用次数: 0

Thermally accelerated Heck reaction under direct mechanocatalysis using palladium milling balls† 用钯磨球直接机械催化热加速Heck反应。

RSC Mechanochemistry Pub Date : 2025-05-13 DOI: 10.1039/D5MR00032G

Johanna Templ, Suhmi Hwang, Tino Schwemin, Hakan Baltaci and Lars Borchardt

引用次数: 0

Mechanochemically micronised Na/NaCl; a superfine reductant† 机械化学微粉化Na/NaCl；超细还原剂†

RSC Mechanochemistry Pub Date : 2025-05-09 DOI: 10.1039/D5MR00039D

Laura E. English, Ross A. Jackson, Nicholas J. Evans, Dawid J. Babula, Harvey J. Draper, Sarah R. Brown, Joseph Fletcher, David J. Liptrot and Kyle G. Pearce

引用次数: 0

Calorimetric determination of the heat capacity function and absolute entropy of yttrium borohydride (Y(BH4)3) mechanochemically prepared 用量热法测定机械化学制备的硼氢化钇（Y(BH4)3）的热容函数和绝对熵

RSC Mechanochemistry Pub Date : 2025-05-06 DOI: 10.1039/D4MR00124A

Konrad Burkmann, Franziska Habermann, Bianca Störr, Jürgen Seidel, Roman Gumeniuk, Klaus Bohmhammel and Florian Mertens

{"title":"Calorimetric determination of the heat capacity function and absolute entropy of yttrium borohydride (Y(BH4)3) mechanochemically prepared","authors":"Konrad Burkmann, Franziska Habermann, Bianca Störr, Jürgen Seidel, Roman Gumeniuk, Klaus Bohmhammel and Florian Mertens","doi":"10.1039/D4MR00124A","DOIUrl":"https://doi.org/10.1039/D4MR00124A","url":null,"abstract":"Over the last two decades, complex metal hydrides have attracted attention in various fields such as chemical hydrogen storage, solid state electrolytes and superconductivity. In this context, we determined thermodynamic properties of the complex metal hydride Y(BH4)3. Yttrium borohydride was prepared by solid state metathesis yielding a mixture containing three equivalents lithium chloride beside the boranate. The benefit of the mechanochemical preparation procedure compared to the classical wet chemical one is to avoid the desolvation step which can lead to a partial decomposition of the hydride. The heat capacity of the compound as a function of the temperature covering a temperature range from 2 K to 370 K was determined using two different calorimetric techniques. Based on the heat capacity data, the standard entropy at 298.15 K was obtained. From the evaluation of the low temperature heat capacity region the Sommerfeld coefficient and the Debye temperature were derived.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 4","pages":" 563-572"},"PeriodicalIF":0.0,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00124a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144524453","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

Preparation of lead dodecyl sulfate nanorod materials mediated by mechanochemistry and green solvent-free catalytic synthesis of heterocyclic derivatives† 机械化学介导十二烷基硫酸铅纳米棒材料的制备及绿色无溶剂催化合成杂环衍生物

RSC Mechanochemistry Pub Date : 2025-05-06 DOI: 10.1039/D4MR00123K

Zhiqiang Wu, Yuan Min, Yongqin Li, Fang Qian, Lin-an Cao, Rong Tan, Enke Feng, Jiya Ding and Pengxi Jiang

{"title":"Preparation of lead dodecyl sulfate nanorod materials mediated by mechanochemistry and green solvent-free catalytic synthesis of heterocyclic derivatives†","authors":"Zhiqiang Wu, Yuan Min, Yongqin Li, Fang Qian, Lin-an Cao, Rong Tan, Enke Feng, Jiya Ding and Pengxi Jiang","doi":"10.1039/D4MR00123K","DOIUrl":"https://doi.org/10.1039/D4MR00123K","url":null,"abstract":"In this work, the lead dodecyl sulfate material (Pb(DS)2) was successfully synthesized for the first time via a mechanochemical ball milling method. The synthesized material was comprehensively analyzed using scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS) and nuclear magnetic resonance (NMR) spectroscopy. The results demonstrate that the Pb(DS)2 catalyst, synthesized via solvent-free mechanical ball milling, possesses a distinctive solid nanorod morphology. Furthermore, the catalyst efficiently promotes the synthesis of heterocyclic derivatives in a solvent-free environment within 20 minutes, achieving a target product yield of up to 98%. Specifically, it produced bis(indolyl)methane derivatives with yields ranging from 78% to 98%, and quinoxaline derivatives with yields ranging from 87% to 98% within the same timeframe. The Pb(DS)2 catalyst also exhibits remarkable catalytic activity in the Biginelli reaction. Notably, the catalyst maintains excellent and stable performance over eight recycling cycles.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 4","pages":" 584-597"},"PeriodicalIF":0.0,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00123k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144524490","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