RSC Mechanochemistry最新文献_第5页

Polymorphism control of polyethylene terephthalate (PET) degradation product via mechanochemistry leads to accelerated microbial degradation† 通过机械化学控制聚对苯二甲酸乙二酯（PET）降解产物的多态性，加速微生物降解†。

RSC Mechanochemistry Pub Date : 2024-08-30 DOI: 10.1039/D4MR00060A

Deepika Shingwekar, Nicholas Lutz, Delbert S. Botes, Elani J. Cabrera-Vega, Gonzalo Campillo-Alvarado, Jay L. Mellies and Jesus Daniel Loya

{"title":"Polymorphism control of polyethylene terephthalate (PET) degradation product via mechanochemistry leads to accelerated microbial degradation†","authors":"Deepika Shingwekar, Nicholas Lutz, Delbert S. Botes, Elani J. Cabrera-Vega, Gonzalo Campillo-Alvarado, Jay L. Mellies and Jesus Daniel Loya","doi":"10.1039/D4MR00060A","DOIUrl":"https://doi.org/10.1039/D4MR00060A","url":null,"abstract":"Widespread usage of single-use plastics such as polyethylene terephthalate (PET) has heavily contributed to a global plastic pollution crisis, necessitating the improvement and development of recycling methods. We previously established a chemo-microbial degradation process for post-consumer PET plastic, consisting of PET depolymerization to form bis(2-hydroxyethyl) terephthalate (BHET) followed by the complete degradation of BHET by a bacterial consortium found to synergistically degrade PET and BHET. The BHET produced during PET depolymerization consists of two polymorphic forms, the α and δ forms. This work investigates the effect of BHET polymorphism on microbial degradation to further optimize the chemo-microbial process. Reversible interconversion methods for BHET polymorphs were effectively developed using mechanochemistry, achieving pure α and δ forms by modulating milling conditions. When inoculated with the bacterial consortium, the α form was degraded faster than the δ form, indicating solid polymorphism is a significant factor for the biodegradation level. This work paves the way to optimize the chemo-microbial process for an increased degradation rate of post-consumer PET and furthers the effort for sustainable plastic recycling methods.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 514-519"},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/mr/d4mr00060a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587685","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

Mechanochemical synthesis of fluorinated perovskites KCuF3 and KNiF3† 氟化包晶 KCuF3 和 KNiF3† 的机械化学合成

RSC Mechanochemistry Pub Date : 2024-08-28 DOI: 10.1039/D4MR00037D

Davide Ceriotti, Piergiorgio Marziani, Federico Maria Scesa, Arianna Collorà, Claudia L. Bianchi, Luca Magagnin and Maurizio Sansotera

{"title":"Mechanochemical synthesis of fluorinated perovskites KCuF3 and KNiF3†","authors":"Davide Ceriotti, Piergiorgio Marziani, Federico Maria Scesa, Arianna Collorà, Claudia L. Bianchi, Luca Magagnin and Maurizio Sansotera","doi":"10.1039/D4MR00037D","DOIUrl":"https://doi.org/10.1039/D4MR00037D","url":null,"abstract":"A solvent-free mechanochemical synthesis of two fluorinated perovskites, KCuF3 and KNiF3, including the optimization of milling time at constant rotational speed, was studied as a practical and green alternative to the classical solvothermal synthesis. The presence of KCuF3 and KNiF3 in the desired crystalline phase as the main product was observed after 6 h of milling. At higher milling times K2CuF4 and K2NiF4 were detected as additional crystalline phases for the Cu- and Ni- based perovskites, respectively. The fluorinated perovskites were characterized by using X-Ray Powder Diffraction (XRD), X-Ray Photoelectron Spectroscopy (XPS) and Scanning Electron Microscopy (SEM), confirming the selective formation of the fluorinated perovskites. The mechanochemical route was also compared to a new mild solvothermal method. An evaluation of the environmental impact and the energy efficiency was performed; moreover, the effectiveness of the mechanochemical process was compared to that of the solvothermal method. The promising results obtained from this innovative method opened the door to the use of solvent-free mechanochemical syntheses as a suitable approach in the field of crystal engineering also.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 520-530"},"PeriodicalIF":0.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/mr/d4mr00037d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587686","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

Cyanation of aryl halides using potassium hexacyanoferrate(ii) via direct mechanocatalysis† 通过直接机械催化使用六氰合铁酸钾（ii）对芳基卤化物进行氰化反应†。

RSC Mechanochemistry Pub Date : 2024-08-27 DOI: 10.1039/D4MR00054D

Suhmi Hwang, Phil M. Preuß, Wilm Pickhardt, Sven Grätz and Lars Borchardt

引用次数: 0

Thermodynamic limits of the depolymerization of poly(olefin)s using mechanochemistry† 利用机械化学法解聚聚（烯烃）的热力学极限。

RSC Mechanochemistry Pub Date : 2024-08-26 DOI: 10.1039/D4MR00079J

Yuchen Chang, Van Son Nguyen, Adrian H. Hergesell, Claire L. Seitzinger, Jan Meisner, Ina Vollmer, F. Joseph Schork and Carsten Sievers

{"title":"Thermodynamic limits of the depolymerization of poly(olefin)s using mechanochemistry†","authors":"Yuchen Chang, Van Son Nguyen, Adrian H. Hergesell, Claire L. Seitzinger, Jan Meisner, Ina Vollmer, F. Joseph Schork and Carsten Sievers","doi":"10.1039/D4MR00079J","DOIUrl":"10.1039/D4MR00079J","url":null,"abstract":"Mechanochemistry is a promising approach for chemical recycling of commodity plastics, and in some cases depolymerization to the monomer(s) has been reported. However, while poly(olefin)s comprise the largest share of global commodity plastics, mechanochemical depolymerization of these polymers in standard laboratory-scale ball mill reactors suffers from slow rates. In this work, the observed reactivities of poly(styrene), poly(ethylene) and poly(propylene) are rationalized on the basis of thermodynamic limitations of their depolymerization by depropagation of free radical intermediates. In addition, subsequent phase partitioning equilibria for the removal of monomers from the reactor via a purge gas stream are discussed for these polymers. For poly(styrene), a typical vibratory ball mill supplies just enough energy for its depolymerization to be driven by either thermal hotspots or adiabatic compression of the impact site, but the same energy supply is far from sufficient for poly(propylene) and poly(ethylene). Meanwhile, removal of styrene from the reactor is thermodynamically hindered by its lower volatility, but this is not an issue for either propylene or ethylene. The implications of these thermodynamic limitations for mechanochemical reactor design and potential for mechanocatalytic processes are highlighted.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 504-513"},"PeriodicalIF":0.0,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11388944/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142305505","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

Single-molecule force spectroscopy shows that side chain interactions govern the mechanochemical response of polypeptide α-helices and prevent the formation of β-sheets† 单分子力谱分析表明，侧链相互作用控制了多肽α-螺旋的机械化学反应，并阻止了β-片†的形成

RSC Mechanochemistry Pub Date : 2024-08-26 DOI: 10.1039/D4MR00068D

Marie Asano, Damien Sluysmans, Nicolas Willet, Colin Bonduelle, Sébastien Lecommandoux and Anne-Sophie Duwez

{"title":"Single-molecule force spectroscopy shows that side chain interactions govern the mechanochemical response of polypeptide α-helices and prevent the formation of β-sheets†","authors":"Marie Asano, Damien Sluysmans, Nicolas Willet, Colin Bonduelle, Sébastien Lecommandoux and Anne-Sophie Duwez","doi":"10.1039/D4MR00068D","DOIUrl":"https://doi.org/10.1039/D4MR00068D","url":null,"abstract":"Secondary α-helix and β-sheet structures are key scaffolds around which the rest of the residues condense during protein folding. Despite their key role in numerous processes to maintain life, little is known about their properties under force. Their stability under mechanical stress, as constantly experienced in the turbulent environment of cells, is however essential. Here, we designed and synthesized two pH-responsive polypeptides, poly(L-glutamic acid) and poly(L-lysine), for single-molecule mechanochemistry experiments using AFM to probe the mechanical unfolding of α-helix and β-sheet secondary motifs. The force experiments, supported by simulations, reveal a superior mechanical stability of the poly(L-lysine) α-helix, which we attribute to hydrophobic interactions of the alkyl side chains. Most importantly, our results show that these interactions play a key role in inhibiting the formation of a metastable β-sheet-like structure when the polypeptide is subjected to mechanical deformations, which might have important implications in the mechanism behind polyQ diseases.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 1","pages":" 37-44"},"PeriodicalIF":0.0,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/mr/d4mr00068d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976284","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

Efficient mechanochemistry of beta blockers: neutralization, salification, and effect of liquid additives† β-受体阻滞剂的高效机械化学：中和、盐化和液体添加剂的影响†。

RSC Mechanochemistry Pub Date : 2024-08-19 DOI: 10.1039/D4MR00078A

Delbert S. Botes, Jesus Daniel Loya, Mahboubeh Ghahremani, Bailee B. Newham, Mikaela I. Aleman, Gary C. George, Daniel K. Unruh and Kristin M. Hutchins

{"title":"Efficient mechanochemistry of beta blockers: neutralization, salification, and effect of liquid additives†","authors":"Delbert S. Botes, Jesus Daniel Loya, Mahboubeh Ghahremani, Bailee B. Newham, Mikaela I. Aleman, Gary C. George, Daniel K. Unruh and Kristin M. Hutchins","doi":"10.1039/D4MR00078A","DOIUrl":"https://doi.org/10.1039/D4MR00078A","url":null,"abstract":"Beta blockers are a class of ubiquitous cardiovascular drugs that have collectively received little attention from a crystal engineering standpoint. Here, we describe the use of mechanochemistry in the salification of five beta blockers (propranolol, metoprolol, acebutolol, atenolol, and labetalol) with nicotinic and isonicotinic acid. Firstly, liquid assisted grinding (LAG) was used to neutralize the commercial beta blocker salts, enabling the efficient gram-scale formation of the free bases, which are essential for cocrystallization. Thereafter, 1 : 1 mechanochemical cocrystallizations were successful in all but one case and nine salts were characterized, eight of which are novel. Furthermore, the racemic free base crystal structure of acebutolol is reported for the first time, as well as the first multicomponent crystal of labetalol that is not a simple salt. Salification was enabled by the large pKa differences between the components, which facilitated the protonation of the basic amine on the beta blockers' alkanolamine skeleton. Thereafter, charge-assisted hydrogen bonding promoted cocrystallization. We envisage salification to be applicable to any beta blocker, considering the current study encompasses approximately one quarter of this drug class. Lastly, the role of different liquid additives in the LAG process was assessed, and the solvent identity was found to play a substantial role in the mechanochemical outcome, although it did not strictly correlate with polarity. This study demonstrates that LAG screening with a wide selection of solvents provides a path to achieve full conversion to products, explore the crystal landscape of multicomponent crystals, and assist in identifying additional phases and/or late stage polymorphs in solid form development.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 492-503"},"PeriodicalIF":0.0,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/mr/d4mr00078a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587684","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

Direct arylation of alkyl fluorides using in situ mechanochemically generated calcium-based heavy Grignard reagents† 使用原位机械化学生成的钙基重格氏试剂对烷基氟化物进行直接芳基化处理†。

RSC Mechanochemistry Pub Date : 2024-08-13 DOI: 10.1039/D4MR00067F

Pan Gao, Julong Jiang, Yamato Fukuzawa, Satoshi Maeda, Koji Kubota and Hajime Ito

引用次数: 0

Rapid and efficient mechanosynthesis of alkali and alkaline earth molybdates† 碱和碱土钼酸盐的快速高效机械合成†。

RSC Mechanochemistry Pub Date : 2024-08-12 DOI: 10.1039/D4MR00042K

Andres Lara-Contreras, Patrick Julien, Jennifer Scott and Emily C. Corcoran

{"title":"Rapid and efficient mechanosynthesis of alkali and alkaline earth molybdates†","authors":"Andres Lara-Contreras, Patrick Julien, Jennifer Scott and Emily C. Corcoran","doi":"10.1039/D4MR00042K","DOIUrl":"https://doi.org/10.1039/D4MR00042K","url":null,"abstract":"Complex molybdates are traditionally prepared via solid-state synthesis and aqueous chemistry methods, which generally require long reaction times and large solvent volumes or high sintering temperatures. However, these techniques often result in undesired secondary species, incomplete reactions, and relatively low yields. Mechanochemistry has proven effective for the synthesis of complex molybdates. This work expands on the development of the mechanochemical synthesis of various heptamolybdates (i.e., sodium, rubidium, and cesium), and trimolybdates (i.e., sodium, rubidium, cesium, strontium, and barium). The obtained materials were characterized via powder X-ray diffraction, Fourier-transform infrared spectroscopy, Raman spectroscopy, thermo-gravimetric analysis, and scanning electron microscopy to assess the purity, morphology, and quality of the sample. High purity samples of the various trimolybdates and heptamolybdates were obtained in less than three hours of reaction time, with minimal energy input and by-products. Mechanochemistry provides a fast, more sustainable, and simple procedure for the synthesis of a wide variety of both trimolybdates and heptamolybdates including the monohydrate form of sodium trimolybdate instead of the trihydrate variant commonly obtained from aqueous reactions.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 477-485"},"PeriodicalIF":0.0,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/mr/d4mr00042k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587682","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

Solvent-free mechanochemical synthesis of azo dyes† 偶氮染料的无溶剂机械化学合成技术†。

RSC Mechanochemistry Pub Date : 2024-08-09 DOI: 10.1039/D4MR00053F

Lin Zhang, Qinglang Song, Yanxian Wang, Rui Chen, Yu Xia, Bin Wang, Weiwei Jin, Shaofeng Wu, Ziren Chen, Azhar Iqbal, Chenjiang Liu and Yonghong Zhang

引用次数: 0

Ball milling assisted mechano-catalytic dye degradation using SrTiO3 nanoparticles† 使用 SrTiO3 纳米粒子进行球磨辅助机械催化染料降解†。

RSC Mechanochemistry Pub Date : 2024-08-09 DOI: 10.1039/D4MR00047A

Aman Shukla, Akshay Gaur, Shivam Dubey and Rahul Vaish

{"title":"Ball milling assisted mechano-catalytic dye degradation using SrTiO3 nanoparticles†","authors":"Aman Shukla, Akshay Gaur, Shivam Dubey and Rahul Vaish","doi":"10.1039/D4MR00047A","DOIUrl":"https://doi.org/10.1039/D4MR00047A","url":null,"abstract":"Ball milling stands as a versatile and widely used technique that involves the mechanical grinding of solid materials via ball mills. Conventionally employed for synthesizing nanomaterials and complex compounds, this method has now been harnessed directly for catalysis due to its capability for surface charge separation. Herein, in the present study, we have explored the potential of ball milling to activate material with low piezoelectric coefficient for catalysis by demonstrating the ball-milling-induced mechano-catalytic activity of SrTiO3 (STO) nanoparticles for the degradation of toxic methylene blue (MB) dye. With the assistance of ball milling, STO nanoparticles (of 0.3 g dosage) were found capable of degrading 70% of 10 ppm MB dye at 400 rpm speed with 10 Zr balls in just 1 hour. A series of parametric studies were performed to analyze the effect of various process conditions, like catalyst dosage, initial concentration of dye, ball milling speed, and number of milling balls. Further, scavenging tests were carried out to detect the responsible reactive species for dye degradation. Moreover, the present ball milling process was compared with the trivial ultrasonication method where STO showed just 12% degradation in 1 hour. The results manifest the superiority of ball milling catalysis which not only offers precise control over reaction parameters but also encompasses scalability, simplicity, and better potential to conduct catalysis under environmentally benign conditions.","PeriodicalId":101140,"journal":{"name":"RSC Mechanochemistry","volume":" 5","pages":" 465-476"},"PeriodicalIF":0.0,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/mr/d4mr00047a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587681","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