The synthesis of metal-organic frameworks (MOFs) is often complex and the desired structure is not always obtained. In this work, we report a methodology that uses a joint machine learning and experimental approach to optimize the synthesis conditions of Al-PMOF (Al2(OH)2TCPP) [H2TCPP = meso-tetra(4-carboxyphenyl)porphine], a promising material for carbon capture applications. Al-PMOF was previously synthesized using a hydrothermal reaction, which gave a low throughput yield due to its relatively long reaction time (16 hours). Here, we use a genetic algorithm to carry out a systematic search for the optimal synthesis conditions and a microwave-based high-throughput robotic platform for the syntheses. We show that, in just two generations, we could obtain excellent crystallinity and yield close to 80% in a much shorter reaction time (50 minutes). Moreover, by analyzing the failed and partially successful experiments, we could identify the most important experimental variables that determine the crystallinity and yield.
Blood transfusions are a life-saving procedure since they can preserve the body’s oxygen levels in patients suffering from acute trauma, undergoing surgery, receiving chemotherapy or affected by severe blood disorders....
The synthesis of metal-organic frameworks (MOFs) is often complex and the desired structure is not always obtained. In this work, we report a methodology that uses a joint machine learning and experimental approach to obtain the optimal synthesis of a MOF. A synthetic conditions finder was used to derive the experimental protocols and a microwave based high-throughput robotic platform was used for the synthesis of Al-PMOF ([H2TCPP[AlOH]2(DMF3(H2O)2)]). Al-PMOF was previously synthesized using a hydrothermal reaction, which gave a low throughput yield due to its relatively long reaction time (16 hours). In this work, we carried out a systematic search for the optimal reaction conditions using a microwave assisted reaction synthesis. For this search we used a genetic algorithm and we show that already in the 2nd generation we obtained conditions that give excellent crystallinity and yield close to 80% in much shorter reaction time (50 minutes). In addition, by analysing the failed and partly successful experiments, we could identify the most important experimental variables that determine the crystallinity and yield.
Blood transfusions are a life-saving procedure since they can preserve the body’s oxygen levels in patients suffering from acute trauma, undergoing surgery, receiving chemotherapy or affected by severe blood disorders. Due to the central role of haemoglobin (Hb) in oxygen transport, the so-called Hb-based oxygen carriers (HBOCs) are currently being developed for situations where donor blood is not available. In this context, an important challenge to be addressed is the oxidation of Hb into methaemoglobin (metHb) which is unable to bind and release oxygen. Since within red blood cells, this process is prevented by a set of protective enzymes such as superoxide dismutase and catalase, several research groups have considered incorporating these enzymes to create HBOCs with antioxidant properties. However, the use of biological enzymes has important limitations related to their high cost, potential immunogenicity or low stability in vivo. Thus, nanomaterials with enzyme-like properties (i.e., nanozymes (NZs)) have emerged as a promising alternative. In this work, we evaluate the antioxidant properties of gold (Au)-based NZs following incorporation within a type of HBOC previously reported by our group (i.e., Hb-loaded metal organic framework (MOF)-based nanocarriers (NCs)). We first prepare Au-loaded Au@MOF-NCs and demonstrate their ability to catalytically deplete two prominent reactive oxygen species (ROS) (i.e., hydrogen peroxide and superoxide radical) which exacerbate Hb’s autoxidation. Furthermore, these catalytic properties are retained over several cycles. Following loading with Hb, we show how the ROS-scavenging properties resulting from the Au-based NZs, translate into a decrease in metHb content. All in all, these results highlight the potential of NZs to create novel HBOCs with antioxidant protection which may find applications as a blood substitute in the future.
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