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Volcano plots, stemming from the Sabatier principle, visualize descriptor-performance relationships, allowing rational catalyst design. Manually drawn volcanoes originating from experimental studies are potentially prone to human bias as no guidelines or metrics exist to quantify the goodness of fit. To address this limitation, we introduce a framework called SPOCK (systematic piecewise regression for volcanic kinetics) and validate it using experimental data from heterogeneous, homogeneous, and enzymatic catalysis to fit volcano-like relationships. We then generalize this approach to DFT-derived volcanoes and evaluate the tool's robustness against noisy kinetic data and in identifying false-positive volcanoes, i.e., cases where studies claim a volcano-like relationship exists, but such correlations are not statistically significant. Once the SPOCK's functional features are established, we demonstrate its potential to identify descriptor-performance relationships, exemplified via the ceria-promoted water-gas shift and single-atom-catalyzed electrocatalytic carbon dioxide reduction reactions. In both cases, the model uncovers descriptors previously unreported, revealing insights that are not easily recognized by human experts. Finally, we showcase SPOCK's capabilities to formulate multivariable descriptors, an emerging topic in catalysis research. Our work pioneers an automated and standardized tool for volcano plot construction and validation, and we release the model as an open-source web application for greater accessibility and knowledge generation in catalysis.
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http://dx.doi.org/10.1021/acscatal.5c00412 | DOI Listing |
ACS Catal
May 2025
Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland.
Volcano plots, stemming from the Sabatier principle, visualize descriptor-performance relationships, allowing rational catalyst design. Manually drawn volcanoes originating from experimental studies are potentially prone to human bias as no guidelines or metrics exist to quantify the goodness of fit. To address this limitation, we introduce a framework called SPOCK (systematic piecewise regression for volcanic kinetics) and validate it using experimental data from heterogeneous, homogeneous, and enzymatic catalysis to fit volcano-like relationships.
View Article and Find Full Text PDFNeural Netw
December 2024
School of Computer and Electronic Information, Guangxi University, Nanning, China; Guangxi Key Laboratory of Multimedia Communications and Network Technology, Guangxi University, Nanning, China.
Local feature extraction plays a crucial role in numerous critical visual tasks. However, there remains room for improvement in both descriptors and keypoints, particularly regarding the discriminative power of descriptors and the localization precision of keypoints. To address these challenges, this study introduces a novel local feature extraction pipeline named OSDFeat (Object and Spatial Discrimination Feature).
View Article and Find Full Text PDFJ Comput Aided Mol Des
May 2005
Bristol-Myers Squibb, 5 Research Parkway, Wallingford, CT 06492, USA.
The dynamic nature and comparatively young age of computational chemistry is such that novel algorithms continue to be developed at a rapid pace. Such efforts are often wrought at the expense of extensive experimental validations of said techniques, preventing a deeper understanding of their potential utility and limitations. Here we address this issue for ligand-based virtual screening descriptors through design of validation experiments that better reflect the aims of real world application.
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