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      Advanced Mechanochemistry Device for Sustainable Synthetic Processes

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          Abstract

          Mechanochemistry is an alternative for sustainable solvent-free processes that has taken the big step to become, in the near future, a useful synthetic method for academia and the fine chemical industry. The apparatus available, based on ball milling systems possessing several optimizable variables, requires too many control and optimization experiments to ensure reproducibility, which has limited its widespread utilization so far. Herein, we describe the development of an automatic mechanochemical single-screw device consisting of an electrical motor, a drill, and a drill chamber. The applicability and versatility of the new device are demonstrated by the implementation of di- and multicomponent chemical reactions with high reproducibility, using mechanical action exclusively. As examples, chalcones, dihydropyrimidinones, dihydropyrimidinethiones, pyrazoline, and porphyrins, were synthesized with high yields. The unprecedented sustainability is demonstrated by comparison of EcoScale and E-factor values of these processes with those previously described in the literature.

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          Most cited references34

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          Ball milling in organic synthesis: solutions and challenges.

          During the last decade numerous protocols have been published using the method of ball milling for synthesis all over the field of organic chemistry. However, compared to other methods leaving their marks on the road to sustainable synthesis (e.g. microwave, ultrasound, ionic liquids) chemistry in ball mills is rather underrepresented in the knowledge of organic chemists. Especially, in the last three years the interest in this technique raised continuously, culminating in several high-quality synthetic procedures covering the whole range of organic synthesis. Thus, the present tutorial review will be focused on the highlights using this method of energy transfer and energy dissipation. The central aim is to motivate researchers to take notice of ball mills as chemical reactors, implementing this technique in everyday laboratory use and thus, pave the ground for future activities in this interdisciplinary field of research.
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            The E factor 25 years on: the rise of green chemistry and sustainability

            The global impact of green chemistry and sustainability and the pivotal role of the E factor concept, over the last twenty five years, is reviewed. The global impact, over the last 25 years, of the principles of green chemistry and sustainability, and the pivotal role of the E factor concept in driving resource efficiency and waste minimisation, in the chemical and allied industries, is reviewed. Following an introduction to the origins of green chemistry and the E factor concept, the various metrics for measuring greenness are discussed. It is emphasised that mass-based metrics such as atom economy, E factors and process mass intensity (PMI) need to be supplemented by metrics, in particular life cycle assessment, which measure the environmental impact of waste and, in order to assess sustainability, by metrics which measure economic viability. The role of catalysis in waste minimisation is discussed and illustrated with examples of green catalytic processes such as aerobic oxidations of alcohols, catalytic C–C bond formation and olefin metathesis. Solvent losses are a major source of waste in the pharmaceutical and fine chemical industries and solvent reduction and replacement strategies, including the possible use of neoteric solvents, such as ionic liquids and deep eutectic solvents, are reviewed. Biocatalysis has many benefits in the context of green and sustainable chemistry and this is illustrated with recent examples in the synthesis of active pharmaceutical ingredients. The importance of the transition from an unsustainable economy based on fossil resources to a sustainable bio-based economy is delineated, as part of the overarching transition from an unsustainable linear economy to a truly green and sustainable circular economy based on resource efficiency and waste minimisation by design.
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              Mechanochemistry: A Force of Synthesis

              The past decade has seen a reawakening of solid-state approaches to chemical synthesis, driven by the search for new, cleaner synthetic methodologies. Mechanochemistry, i.e., chemical transformations initiated or sustained by mechanical force, has been advancing particularly rapidly, from a laboratory curiosity to a widely applicable technique that not only enables a cleaner route to chemical transformations but offers completely new opportunities in making and screening for molecules and materials. This Outlook provides a brief overview of the recent achievements and opportunities created by mechanochemistry, including access to materials, molecular targets, and synthetic strategies that are hard or even impossible to access by conventional means.
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                Author and article information

                Journal
                ACS Omega
                ACS Omega
                ao
                acsodf
                ACS Omega
                American Chemical Society
                2470-1343
                08 May 2020
                19 May 2020
                : 5
                : 19
                : 10868-10877
                Affiliations
                []University of Coimbra, CQC, Department of Chemistry , Rua Larga, 3004-535 Coimbra, Portugal
                []LEDAP, Departamento de Engenharia Mecânica, FCT-Universidade de Coimbra , Polo II, 3030-194 Coimbra, Portugal
                [§ ]Faculty of Pharmacy, Exact Sciences and Technology Unit, State University of Goias , 75132400 Anapolis, Goias, Brazil
                Author notes
                [* ]Email: mmpereira@ 123456qui.uc.pt . Tel: +351919853716. Fax: +351239852080.
                [* ]Email: mpineiro@ 123456qui.uc.pt . Tel: +351239854479. Fax: +351239852080.
                Article
                10.1021/acsomega.0c00521
                7240818
                29a12271-ce41-4c2c-8d34-174a84f0e8fe
                Copyright © 2020 American Chemical Society

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

                History
                : 05 February 2020
                : 03 April 2020
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                ao0c00521

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