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The Changing Landscape of Materials Discovery
Get PDFIn this perspective, we will discuss the impact of some of the most recent advancements in materials discovery, particularly focusing on the role of robotics, artificial intelligence, and self-driving laboratories, as well as their implications for the Swiss research landscape. While it seems timely to aim for broad, revolutionary breakthroughs in this field, we argue that more incremental steps – such as, for example, fully automatic grinding of solid powders or fully automated Rietveld refinements – may have a more significant impact on materials discovery, at least in the short run. In the center of these considerations is how small, interdisciplinary groups can drive significant progress by contributing targeted innovations, such as e.g.robotic sample preparation or computational predictions. Additionally, given the large investments that are necessary for future infrastructures in materials discovery, we discuss the potential case for the establishment – in the long run – of a national infrastructure, a Swiss Materials Discovery Lab, to support automated material synthesis and advanced characterization, ultimately accelerating innovation in both academic and industrial settings
Operando Nuclear Magnetic Resonance (NMR) Studies of a Trickle-bed Reactor Using D-T2 Correlations
Get PDFCatalytic conversions in fine-chemical and pharmaceutical production are increasingly performed in trickle-bed rectors. Optimisation of these processes is usually based on end of pipe measurement made at specific residence times. This process is both time-consuming and the data sometimes challenging to interpret. In the present work, operando nuclear magnetic resonance (NMR) techniques both at the scale of the whole bed (global) and spatially resolved within the bed (local) are used to gain new insights into the catalytic conversion process under reaction conditions. Spatially resolved spectroscopic and diffusion-T2-relaxation (D-T2) methods interrogate local differences in chemical conversion and selectivity, and mass transport (molecular self-diffusion) respectively, thereby providing valuable information for process simulation models. This capability is demonstrated using the continuous flow three phase (gas-liquid-solid) hydrogenation of benzonitrile over a fixed bed of 0.5 wt% Pd/Al2O3 catalyst pellets yielding toluene and benzylamine. Global 1H spectroscopic and D-T2 were used to monitor chemical conversion and the approach to steady state; these were subsequently followed by spatially resolved 1H spectra and spatially resolved D-T2 correlations to examine the local differences in axial conversion and selectivity of the catalyst bed packing. At steady-state a global conversion of 63% was achieved with 65% and 25% selectivity to benzylamine and toluene respectively. Heterogeneities in the local (axial) conversion and selectivity differed by 31% along the total catalyst bed length. These techniques should be applicable to many three-phase heterogeneous catalytic systems provided that the T2 relaxation time of the reactants and products is not prohibitively small
Modeling-based Approach Towards Quality by Design for a Telescoped Process
Get PDFA telescoped, two-step synthesis was investigated by applying Quality by Design principles. A kinetic model consisting of 12 individual reactions was successfully established to describe the synthesis and side reactions. The resulting model predicts the effects of changes in process parameters on total yield and quality. Contour plots were created by varying process parameters and displaying the model predicted process response. The areas in which the process response fulfils predetermined quality requirements are called design spaces. New ranges for process parameters were explored within these design spaces. New conditions were found that increased the robustness of the process and allowed for a considerable reduction of the used amounts of a reagent. Further optimizations, based on the newly generated knowledge, are expected. Improvements can either be direct process improvements or enhancements to control strategies. The developed strategies can also be applied to other processes, enhancing upcoming and preexisting research and development efforts
Harvesting at Night or During the Day – What Is the Impact on the Sauvignon Blanc\u27s Varietal and Aroma Profiles? Highlights of Analytical Sciences in Switzerland
No full textExtending Droplet-Based Microfluidic Tools to Single-Atom Heterogeneous Catalysis
Get PDFFrom energy-related transformations to organic syntheses, single-atom heterogeneous catalysts (SACs) are offering new prospects to tackle sustainability challenges. However, scarce design guidelines and poor mechanistic understanding due to a lack of discovery and operando characterization tools impede theirbroader development. This perspective offers a glimpse into how droplet-based microfluidic technologies mayhelp solve both of these issues, and provides technical considerations for platform design to systematically fabricate SACs and study them under operational conditions during liquid-phase organic syntheses
Oxidative Defect Detection Within Free and Packed DNA Systems: A Quantum Mechanical/Molecular Mechanics (QM/ MM) Approach
Get PDFBase excision repair enzymes (BERs) detect and repair oxidative DNA damage with efficacy despite the small size of the defects and their often only minor structural impact. A charge transfer (CT) model for rapid scanning of DNA stretches has been evoked to explain the high detection rate in the face of numerous, small lesions. The viability of CT DNA defect detection is explored via hybrid QM/MM computational studies that leverage the accuracy of quantum mechanics (QM) for a region of interest and the descriptive power of molecularmechanics (MM) for the remainder of the system. We find that the presence of an oxidative lesion lowers theredox free energy of oxidation by approximately 1.0 eV regardless of DNA compaction (free DNA versus packed DNA in nucleosome core particles) and damage location indicating the high feasibility of a CT-based process for defect detection in DNA
