Porous aluminosilicates such as zeolites are ubiquitous catalysts for the production of high-value and industrially relevant commodity chemicals, including the conversion of hydrocarbons, amines, alcohols, and others. Bimolecular reactions are an important subclass of reactions that can occur on Brønsted acid sites of a zeolite catalyst. Kinetic modeling of these systems at the process scale requires the interaction energetics of reactants and the active sites to be described accurately. It is generally known that adsorption is a coverage-dependent phenomenon, with lower heats of adsorption observed for molecules at higher coverage. However, few studies have systematically investigated the coadsorption of molecules on a single active site, specifically focusing on the strength of interaction of the second adsorbate after the initial adsorption step. In this work, we quantify the unimolecular and bimolecular adsorption energies of varying adsorbates, including paraffins, olefins, alcohols, amines, and noncondensible gases in the acidic and siliceous ZSM-5 frameworks. As a special case, olefin adsorption was examined for physisorption and chemisorption regimes, characterized by π-complex, framework alkoxide and carbenium ion adsorption, respectively. The effects of functional groups and molecular size were quantified, and correlations that relate the adsorption of the second adsorbate identity to that of the first adsorbate are provided.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1021/acs.jpcb.1c02929 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Environmental applications of metal-organic framework-based three-dimensional macrostructures: a review.
Chem Soc Rev
January 2025
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Sciences, Zhejiang Normal University, Jinhua 321004, P. R. China.
Metal-organic frameworks (MOFs) hold considerable promise for environmental remediation owing to their exceptional performance and distinctive structure. Nonetheless, the practical implementation of MOFs encounters persistent technical hurdles, notably susceptibility to loss, challenging recovery, and potential environmental toxicity arising from the fragility, insolubility, and poor processability of MOFs. MOF-based three-dimensional macrostructures (3DMs) inherit the advantageous attributes of the original MOFs, such as ultra-high specific surface area, tunable pore size, and customizable structure, while also incorporating the intriguing characteristics of bulk materials, including hierarchical structure, facile manipulation, and structural flexibility.
View Article and Find Full Text PDFThe Role of Long-Range Interactions Between High-Entropy Single-Atoms in Catalyzing Sulfur Conversion Reactions.
Adv Mater
January 2025
School of Materials Science and Engineering, University of Science and Technology of China, Shenyang, 110016, China.
Sulfur conversion reactions are the foundation of lithium-sulfur batteries but usually possess sluggish kinetics during practical battery operation. Herein, a high-entropy single-atom catalyst (HESAC) is synthesized for this process. In contrast to conventional dual-atom catalysts that form metal-metal bonds, the center metal atoms in HESAC are not bonded but exhibit long-range interactions at a sub-nanometer distance (<9 Å).
View Article and Find Full Text PDFMetamorphic Proteins to Achieve Conformationally Selective Material Surface Binding.
Small
January 2025
Department of Chemistry, University of Miami, Coral Gables, FL, 33146, USA.
The controlled binding of proteins on nanoparticle surfaces remains a grand challenge required for many applications ranging from biomedical to energy storage. The difficulty in achieving this ability arises from the different functional groups of the biomolecule that can adsorb on the nanoparticle surface. While most proteins can only adopt a single structure, metamorphic proteins can access at least two different conformations, which presents intriguing opportunities to exploit such structural variations for binding to nanoparticles.
View Article and Find Full Text PDFKinetic processes of interfacial transport of reactive species across plasma-water interfaces: the effect of temperature.
Phys Chem Chem Phys
January 2025
Department of Electrical Engineering and Electronics, The University of Liverpool, Brownlow Hill, L69 3GJ, UK.
This work quantifies, through use of molecular dynamics (MD) simulations, the kinetic rates of physical surface processes occurring at a plasma-water interface. The probabilities of adsorption, absorption, desorption and scattering were computed for O, NO, NO, NO, OH, HO, HNO, HNO, and NO as they interact with the interface at three water temperatures: 298 K, 323 K, and 348 K. Species are categorised into the short-residence group (O, NO, NO, and NO) and the long-residence group (OH, HO, HNO, HNO, and NO) based on their mean surface residence time.
View Article and Find Full Text PDFQuality, improvement of soluble dietary fiber from by-products by steam explosion and cellulase modification: Structural and functional analysis.
Food Chem X
January 2025
College of Food Science, Fujian Agriculture and Forestry University, Fuzhou, Fujian, PR China.
Steam explosion (SE) and cellulase treatment are potentially effective processing methods for by-products, for use in high-value applications. The treatment conditions were optimized by response surface methodology, increasing the soluble dietary fiber (SDF) yield by 1.52 and 1.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!