Universal Predictive Power: Introducing the Electronic Structure Decomposition Approach for CO Adsorption and Activation on Al2O3-Supported Ru Nanoparticles.

Accurate prediction of catalyst performance is crucial for designing materials with specific catalytic functions. While the density functional theory (DFT) method is widely used for its accuracy, modeling heterogeneous systems, especially supported transition metals, poses significant computational challenges. To address these challenges, we introduce the Electronic Structure Decomposition Approach (ESDA), a novel method that identifies specific density of states (DOS) areas responsible for adsorbate interaction and activation on the catalyst. As a case study, we investigate the influence of α-Al2O3(0001) as a support material on CO adsorption energy and the stretching frequency of the C-O bond on Ru nanoparticles (NPs). Using multiple linear regression analysis, ESDA models were trained with data from isolated Ru NPs and adjusted using supported NP sample data. The ESDA models accurately predict the CO adsorption energies and C-O vibrational frequencies, demonstrating strong linear correlations between predicted and DFT-calculated values with low errors across various adsorption sites for both isolated and supported Ru NPs. Beyond pinpointing the DOS areas responsible for CO adsorption and C-O bond activation, this study provides insights into manipulating these DOS areas to control CO activation, hence facilitating CO dissociation. Additionally, ESDA significantly accelerates the characterization and prediction of CO adsorption and activation on both isolated and supported Ru NPs compared to DFT calculations, expediting the design of new catalytic materials and advancing catalysis research. Furthermore, ESDA's reliance on the electronic structure as a descriptor suggests its potential for predicting various properties beyond catalysis, broadening its applicability across diverse scientific domains.

Impact of multiple H/D replacements on the physicochemical properties of flurbiprofen.

Although deuterium incorporation into pharmaceutical drugs is an attractive way to expand drug modalities, their physicochemical properties have not been sufficiently examined. This study focuses on examining the changes in physicochemical properties between flurbiprofen (FP) and flurbiprofen-d8 (FP-d8), which was successfully prepared by direct and multiple H/D exchange reactions at the eight aromatic C-H bonds of FP. Although the effect of deuterium incorporation was not observed between the crystal structures of FP and FP-d8, the melting point and heat of fusion of FP-d8 were lower than those of FP. Additionally, the solubility of FP-d8 increased by 2-fold compared to that of FP. Calculation of the interaction energy between FP/FP-d8 and water molecules using the multi-component density functional theory method resulted in increased solubility of FP-d8. These novel and valuable findings regarding the changes in physicochemical properties triggered by deuterium incorporation can contribute to the further development of deuterated drugs.