State Key Laboratory of BioFibers and Eco-Textiles, Institute of Materials for Energy and Environment, College of Materials Science and Engineering, Qingdao University, Qingdao 266071, China.
Published: August 2024
AI Article Synopsis
Article Abstract
Significant interest has emerged for the application of Pd-InO catalysts as high-performance catalysts for CO hydrogenation to CHOH. However, precise active site control in these catalysts and understanding their reaction mechanisms remain major challenges. In this investigation, a series of Pd-InO catalysts were synthesized, revealing three distinct types of active sites: In-O, Pd-O(H)-In, and PdIn. Lower Pd loadings exhibited Pd-O(H)-In sites, while higher loadings resulted in PdIn intermetallic compounds. These variations impacted catalytic performance, with Pd-O(H)-In catalysts showing heightened activity at lower temperatures due to the enhanced CO adsorption and H activation, and PdIn catalysts performing better at elevated temperatures due to the further enhanced H activation. In situ DRIFTS studies revealed an alteration in key intermediates from *HCOO over In-O bonds to *COOH over Pd-O(H)-In and PdIn sites, leading to a shift in the main reaction pathway transition and product distribution. Our findings underscore the importance of active site engineering for optimizing catalytic performance and offer valuable insights for the rational design of efficient CO conversion catalysts.
Loewdin charges from density functional theory calculations were used here to obtain general, univariate linear correlations for the prediction of experimental Hammett parameters and relative reaction rates. While previous studies have established that Hirshfeld and CM5 charges perform strongly as univariate predictors, the near-ubiquitous Loewdin charges have not yet been evaluated. To this end, we assess the predictive capability of Loewdin charges for three chemical systems.
The proliferation of short video apps has brought to the forefront the issue of adolescent addiction, a challenge that resonates across Chinese society. Despite growing attention, a comprehensive understanding of the factors propelling addiction at various adolescent stages and its impact on academic performance remains scarce. This study aims to fill this void by identifying key growth stages and crafting targeted intervention strategies.
Fuel cells have become increasingly important in recent years because of their high energy efficiency and low environmental impact. However, key challenges remain in the widespread adoption of fuel-cell vehicles, including reducing Pt usage in catalysts and improving their durability. In this study, a high-performance Pt@carbon-dot-film core-shell catalyst was successfully synthesized using a nonequilibrium reaction field, , solution plasma (SP) process, by adjusting the electrolyte pH.
Synthetic photobiocatalysts are promising catalysts for valuable chemical transformations by harnessing solar energy inspired by natural photosynthesis. However, the synergistic integration of all of the components for efficient light harvesting, cascade electron transfer, and efficient biocatalytic reactions presents a formidable challenge. In particular, replicating intricate multiscale hierarchical assembly and functional segregation involved in natural photosystems, such as photosystems I and II, remains particularly demanding within artificial structures.
Genetically encoded noncanonical amino acids can introduce new-to-nature activation modes into enzymes. While these amino acids can act as catalysts on their own due to their inherent chemical properties, interactions with adjacent residues in an enzyme, such as those present in natural catalytic dyads or triads, unlock a higher potential for designer enzymes. We incorporated a boron-containing amino acid into the protein scaffold RamR to create an active enzyme for the kinetic resolution of α-hydroxythioesters.
