Navigating Ball Mill Specifications for Theory‐to‐Practice Reproducibility in Mechanochemistry

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(48)

Опубликована: Авг. 16, 2024

Abstract The rising prospects of mechanochemically assisted syntheses hold promise for both academia and industry, yet they face challenges in understanding and, therefore, anticipating respective reaction kinetics. Particularly, dependencies based on variations milling equipment remain little understood globally overlooked. This study aims to address this issue by identifying critical parameters through kinematic models, facilitating the reproducibility mechanochemical reactions across most prominent mills laboratory settings, namely planetary mixer mills. Through a series selected experiments replicating major classes organic, organometallic, transition metal‐catalyzed, inorganic from literature, we rationalize independence kinetics when accumulated energy criterion is met. As step forward facilitate practicability our findings, provide freely accessible online tool [†] that allows calculation different Our work advances current mechanochemistry lays foundation future rational exploration rapidly evolving field.

Язык: Английский

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Shaking Things from the Ground-Up: A Systematic Overview of the Mechanochemistry of Hard and High-Melting Inorganic Materials

Molecules, Год журнала: 2023, Номер 28(2), С. 897 - 897

Опубликована: Янв. 16, 2023

We provide a systematic overview of the mechanochemical reactions inorganic solids, notably simple binary compounds, such as oxides, nitrides, carbides, sulphides, phosphides, hydrides, borides, borane derivatives, and related systems. Whereas solid state has been traditionally considered to be little synthetic value by broader community chemists, solid-state community, in particular researchers focusing on materials, have thrived building rich dynamic research field based mechanically-driven transformations substances typically seen inert high-melting. This review provides an insight into chemical richness and, at same time, offers their tentative categorisation transformation type, resulting seven distinct groupings: (

Язык: Английский

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NMR in operando monitoring of mechanochemically accelerated sublimations

Chem, Год журнала: 2023, Номер 9(5), С. 1318 - 1332

Опубликована: Март 24, 2023

Язык: Английский

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A Greener Pathway to Enantiopurity: Mechanochemical Deracemization through Abrasive Grinding

Chemistry - A European Journal, Год журнала: 2023, Номер 29(35)

Опубликована: Апрель 14, 2023

We report the first case of mechanochemical deracemization by using liquid-assisted abrasive grinding. The target molecule is a precursor Paclobutrazol, an important fungicide and plant growth inhibitor. Using deracemization, we are even able to transform 10 % ee scalemic mixture this latter in enantioenriched product 97 couple hours. This substantially shorter compared solution-based methodologies. present paper thus introduces efficient greener process enantiopure material.

Язык: Английский

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Deriving kinetic insights from mechanochemically synthesized compounds using multivariate analysis (MCR-ALS) of powder X-ray diffraction data

RSC Mechanochemistry, Год журнала: 2024, Номер 1(1), С. 106 - 115

Опубликована: Янв. 1, 2024

Application of MCR-ALS method on PXRD data from ex situ and in experiments, to study the kinetics co-crystallization theophylline malonic acid via mechanochemistry.

Язык: Английский

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Eco-Friendly Production of Hyper-Cross-Linked Polymers Using Mechanosynthesis and Bioresources: A Critical Review

ACS Sustainable Chemistry & Engineering, Год журнала: 2022, Номер 10(49), С. 16090 - 16112

Опубликована: Дек. 2, 2022

Hyper-cross-linked polymers (HCPs) are receiving great attention due to their high specific surface areas, allowing them offer performances in many different applications. However, most of the time, syntheses require hazardous and time-consuming protocols, making implementation scaling up difficult. To overcome this problem, a relatively old technology such as mechanosynthesis (MS) has gained renewed interest greener faster produce HCPs, which involves much lower energy consumption during reaction process. In perspective, latest advances on HCPs based MS protocols compiled analyzed, subdivided into those Friedel–Crafts alkylation, Scholl coupling reactions, other less common procedures. An analysis versus solvent-based regarding 12 principles green chemistry is also reported, well section including summary recent applications HCPs. Finally, use biobased precursors for formulation discussed, thus pooling knowledge greener, faster, more widely applicable future development

Язык: Английский

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The Role of Crystalline Intermediates in Mechanochemical Cyclorhodation Reactions Elucidated by in‐Situ X‐ray Powder Diffraction and Computation

Chemistry - A European Journal, Год журнала: 2023, Номер 29(52)

Опубликована: Июнь 24, 2023

The occurrence of crystalline intermediates in mechanochemical reactions might be more widespread than previously assumed. For example, a recent study involving the acetate-assisted C-H activation N-Heterocycles with [Cp*RhCl2 ]2 by ball milling revealed formation transient cocrystals between reagents prior to step. However, such were only observed through stepwise intervallic ex-situ analysis, and their exact role process remained unclear. In this study, we monitored discrete, stoichiometric benzo[h]quinoline using in-situ synchrotron X-ray powder diffraction. This continuous analysis an initial cocrystal that transformed into second form. Computational studies showed differences noncovalent interactions made unit later-appearing reactive towards NaOAc. demonstrated advantage before metalation-deprotonation step, how net cooperative action weak experiments can lead stable supramolecular assemblies, which enhance substrate under ball-milling conditions. could explain superiority some reactions, as activation, compared solution-based counterparts.

Язык: Английский

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Intermediates in Mechanochemical Reactions

Angewandte Chemie, Год журнала: 2024, Номер 136(14)

Опубликована: Янв. 5, 2024

Abstract Mechanochemical reactions offer methodological and environmental advantages for chemical synthesis, constantly attracting attention within the scientific community. Besides unmistakable sustainability advantages, conditions under which mechanochemical occur, namely solventless conditions, sometimes facilitate isolation of otherwise labile or inaccessible products. Despite these limited knowledge exists regarding mechanisms types intermediates involved. Nevertheless, in an expanding number cases, ex situ monitoring techniques have allowed observation, characterization, reaction transformations. In this Minireview, we present a series examples reactive been detected spanning organic, organometallic, inorganic, materials chemistry. Many were stabilized by non‐covalent interactions, played pivotal role guiding We believe that uncovering understanding such instances, growing mechanochemistry community could find novel opportunities catalysis discover new while achieving simplification design.

Язык: Английский

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Listening to the Formation of Polymorphs in a Ball Mill

Analytical Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 27, 2025

In this contribution, we apply our newly developed ball-milling operando platform, which combines Raman spectroscopy and thermal (IR) imaging, as well acoustic high-speed optical video recordings, to the synthesis transformation of citric acid–isonicotinamide (1:2) cocrystal polymorphs in transparent PMMA jars. Particularly, demonstrate how Raman, temperature, acoustic, data are complementary enable detection connection chemical physical events happening during a time-resolved manner. Importantly, show that formation three can be detected through analyses solely. Even more impressively, meticulous sound allowed subtle polymorphic transitions perceived mode when was not conclusive enough. Such changes signatures greatly linked beads' motions milling jar. A new analysis methodology recordings is proposed combination energetic statistical approaches simplifies for potential users. The interpretation signals further validated thanks videos recorded synchronization with all other techniques. Finally, broaden opaque stainless-steel jars, showing relevance method following transformations cocrystals, pure substances, any type

Язык: Английский

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Kinetics of the mechanochemical transformations in the “glycine - oxalic acid dihydrate” system revisited: The role of water

Frontiers in Chemistry, Год журнала: 2025, Номер 13

Опубликована: Март 25, 2025

Introduction: Kinetics of the mechanochemical transformations in “glycine–oxalic acid dihydrate” system were revisited, order to compare results obtained for ball milling same reactants different ball-milling devices. Methods: The a commercial vibrational mill NARVA Vibrator DDR-GM9458 (ex situ study, this work) compared with previously published studies: ex home-made restricted-impact device and Retsch MM400 mill. Results: We studied effect various factors on under conditions, such as air humidity, frequency mechanical pulses existence induction period, starting glycine polymorph duration period case high-frequency milling, or formation G2O GO two competing products, former dominating at early stage treatment “kinetic”, faster crystallizing phase, latter formed only final thermodynamically stable product after prolonged treatment. Discussion: abovementioned interpreted consistently considering possibility that water released from oxalic crystal hydrate may have significant transformations, even though it does not enter structures bis-glycinium oxalate (G2O) glycinium semioxalate (GO) products.

Язык: Английский

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