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Donaire González, Antonio

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Donaire González, Antonio
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Universidad de Murcia. Departamento de Química Inorgánica
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    Sustainable chemo-enzymatic synthesis of glycerol carbonate (meth)acrylate from glycidol and carbon dioxide enabled by ionic liquid technologies
    (Royal Society of Chemistry, 2021-05-06) Villa Aroca, Rocío; Porcar, Raul; Nieto Cerón, Susana; Donaire González, Antonio; García-Verdugo, Eduardo; Luis, Santiago V.; Lozano Rodríguez, Pedro; Bioquímica y Biología Molecular B e Inmunología; Facultad de Química
    A sustainable chemo-enzymatic process for producing both glycerol carbonate acrylate (GCA) and glycerol carbonate methacrylate (GCMA), as useful monomers for the preparation of biodegradable plastic materials, has been carried out by taking advantage of ionic liquid (IL) technologies. The process consiste of two consecutive catalytic steps, which can be carried out by either sequential or one-pot experimental approaches. Glycidyl (meth)acrylate was firstly synthesized by enzymatic transesterification of (meth)acrylate vinyl ester with glycidol in Sponge Like Ionic Liquids (SLILs) as the reaction medium (100% yield after 6 h at 60 °C). SLILs not only provided a suitable reaction medium, but also allowed the simple isolation of the resulting glycidyl esters as an IL-free pure fraction through a straightforward cooling/centrifugation protocol. The second step consisted of the synthesis of GCA, or GCMA, as the outcome of the cycloaddition of CO2 to the obtained glycidyl acrylate or glycidyl methacrylate, respectively, catalysed by a covalently attached 1-decyl-2-methylimidazolium moiety (Supported Ionic Liquid-Like Phase, SILLP) in a solvent-free system and under mild conditions (60 °C, 1–10 bar), leading to up to 100% yield after 6 h. The components of the reaction system (biocatalyst/SLIL/SILLP) can be fully recovered and reused for atleast 6 cycles with unchanged catalytic performance.
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    Sustainable set-ups for the biocatalytic production and scale-up of panthenyl monoacyl esters under solvent-free conditions
    (American Chemical Society, 2023-03-22) Nieto Cerón, Susana; Bernal Palazón, Juana María; García Verdugo, Eduardo; Donaire González, Antonio; Lozano Rodríguez, Pedro; Villa Aroca, Rocío; Química Inorgánica; Facultades de la UMU::Facultad de Química
    A sustainable scaling-up process for the biocatalytic production of new bioactive provitamin-B5 monoacyl esters has been demonstrated. A solvent-free reaction protocol based on the formation of eutectic mixtures between neat substrates render to highly efficient direct esterification of free fatty acids (i.e. from C6 to C18 alkyl chain length) with panthenol catalyzed by lipase. The scale-up from 0.5 to 500 g was evaluated by means of several reaction systems (i.e. ultrasound-assistance, orbital shaking, rotary evaporator, and mechanical stirring coupled to vacuum). For all reactor systems, the yield in panthenyl monoacyl esters was improved by increasing the length of the alkyl chain of the fatty acid (i.e. from 63 % yield for panthenyl butyrate to 83 % yield for panthenyl myristate). The best results (87 % - 95 % product yield, for all cases) were obtained upon a scale-up (50-500 g size) and when a vacuum system was coupled to the biocatalytic reaction unit. Under the optimized conditions a five-fold reduction of the amount of biocatalyst with respect reactors without vacuum was achieved. The recovery and reuse of the immobilized enzyme for 5 operation cycles was also demonstrated. Finally, different metrics have been applied to assess the greenness of the solvent-free biocatalytic synthesis of panthenyl monoesters here reported.
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    Direct biocatalytic processes for CO2 capture as a green tool to produce value-added chemicals
    (MDPI (Multidisciplinary Digital Publishing Institute), 2023-07-19) Villa Aroca, Rocío; Nieto Cerón, Susana; Donaire González, Antonio; Lozano Rodríguez, Pedro; Bioquímica y Biología Molecular B e Inmunología; Química Inorgánica; Facultad de Química
    Direct biocatalytic processes for CO2 capture and transformation in value-added chemicals may be considered a useful tool for reducing the concentration of this greenhouse gas in the atmosphere. Among the other enzymes, carbonic anhydrase (CA) and formate dehydrogenase (FDH) are two key biocatalysts suitable for this challenge, facilitating the uptake of carbon dioxide from the atmosphere in complementary ways. Carbonic anhydrases accelerate CO2 uptake by promoting its solubility in water in the form of hydrogen carbonate as the first step in converting the gas into a species widely used in carbon capture storage and its utilization processes (CCSU), particularly in carbonation and mineralization methods. On the other hand, formate dehydrogenases represent the biocatalytic machinery evolved by certain organisms to convert CO2 into enriched, reduced, and easily transportable hydrogen species, such as formic acid, via enzymatic cascade systems that obtain energy from chemical species, electrochemical sources, or light. Formic acid is the basis for fixing C1-carbon species to other, more reduced molecules. In this review, the state-of-the-art of both methods of CO2 uptake is assessed, highlighting the biotechnological approaches that have been developed using both enzymes.
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