Article
Medicine, Research & Experimental
Anita Girelli, Christian Beck, Famke Baeuerle, Olga Matsarskaia, Ralph Maier, Fajun Zhang, Baohu Wu, Christian Lang, Orsolya Czakkel, Tilo Seydel, Frank Schreiber, Felix Roosen-Runge
Summary: The study reveals that under different solution conditions, antibodies in high-concentration formulations undergo a transition from a well-dispersed solution to a phase-separated and macroscopically arrested system. Although there is a significant decrease in antibody diffusion, internal flexibility persists to a significant degree, ensuring the preservation of molecular function.
MOLECULAR PHARMACEUTICS
(2021)
Article
Chemistry, Applied
Bihong Li, Pan Huang, Piao Cao, Weiqun Gao, Weizhong Zheng, Cheng Lian, Weizhen Sun, Ling Zhao
Summary: This study investigates the adsorption and diffusion behaviors of C4 reactants on zeolites with different topologies, revealing that the surface area, largest cavity diameter, and pore limiting diameter are crucial structural parameters determining the adsorption and diffusion of C4 reactants. Additionally, the dimensions of zeolitic channels also influence the selectivity of isobutane to butene and the diffusion of C4 reactants.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Engineering, Chemical
Piao Cao, Weizhong Zheng, Weizhen Sun, Ling Zhao
Summary: The study investigated the adsorption and diffusion behaviors of C8 isomers and C9 component as main products of isobutane alkylation catalyzed by zeolites with different topologies. The results showed that the adsorption capacity and molecular diffusion coefficient of zeolites were related to temperature and loading, with catalysts showing high selectivity having larger molecular diffusion coefficients.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Multidisciplinary Sciences
Jiamin Yuan, Zhiqiang Liu, Yimo Wu, Jingfeng Han, Xiaomin Tang, Chengbin Li, Wei Chen, Xianfeng Yi, Jian Zhou, Rajamani Krishna, German Sastre, Anmin Zheng
Summary: Contrary to the general trend, the movement of long-chain molecules slows at higher temperatures under confinement due to the thermal resistance effect. This phenomenon limits molecular transportation in nanoscale channels, as confirmed by zero length column experiments. This study contributes to our understanding of anomalous diffusion and its mechanisms in confined systems.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Dimitris Mitrogiannis, Maria Psychoyou, Ioannis Baziotis, Constantinos Mavrogonatos, Nikolaos Koukouzas, Ioannis Anastopoulos, Marios Fyrillas, Vassilis J. Inglezakis
Summary: This study presents equilibrium and kinetic experiments for the adsorption of PO4-P from aqueous solutions onto sustainable and low-cost modified adsorbents. The kinetics of PO4-P adsorption were analyzed using a dimensionless two-phase homogeneous surface diffusion model (TP-HSDM) and the double selectivity isotherm equation (DSM). The TP-HSDM fit the data well with an average relative error of 14.6% and 17.4% for CaT-Z and CaT-B, respectively. The mass transfer mechanism was found to be intraparticle diffusion for both materials, as indicated by the dimensionless Biot number.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2023)
Article
Chemistry, Applied
Stacey I. Zones, Son-Jong Hwang, Kaustav Chaudhuri, C. -Y. Chen, Jesus Pascual
Summary: In this work, large organo-cations are used to create new structures in the Ge/Si/F synthesis space, based on discoveries by the Corma group at ITQ. Three compositions, SSZ-117, 120, and 121, are patented and characterized. SSZ-117 crystallizes in a layered structure, while SSZ-120 and 121 are believed to have large pores. The influence of the organo-cation in the synthesis product is found to be stronger than that of F.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Physics, Fluids & Plasmas
Luana S. Moreira, Douglas D. de Vargas, Mateus H. Koehler
Summary: This study investigates the effects of introducing flexibility in water force fields on molecular dynamics simulations of nanoconfined water. The results show that viscosity, diffusion, and dipole orientation are greatly influenced by the flexibility and the family of force fields used.
Article
Physics, Fluids & Plasmas
Luana S. Moreira, Douglas D. de Vargas, Mateus H. Kohler
Summary: The introduction of flexibility in water force fields during molecular dynamics simulations of nanoconfined water has a significant impact on viscosity, diffusion, and dipole orientation. The level of confinement and the choice of force-field family greatly influence the behavior of water molecules in nanoconfined systems.
Article
Chemistry, Applied
Zehua Huang, Luyan Huang, Weikun Chen, Jian Jing, Xuefeng Liang, Lisheng Zhang, Yuanzheng Tang, Zhiming Liu, Yan He, Huifang Li
Summary: This study investigates the diffusion behaviors of different gas molecules in the channels of AlPO4-5 zeolite-like material using MD simulations and DFT calculations. The results show that light molecules have more freedom for diffusion at low loading, while heavier molecules are controlled by gas-gas and gas-porous media interactions at high loading.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Alice Pancaldi, Luisa Raimondo, Alessandro Minotto, Adele Sassella
Summary: The ability to control organic thin film properties is crucial for high-performance thin film devices. Post-growth processes can modify the film structure and morphology, affecting device performance. Understanding and addressing these processes is essential for controlling film properties.
Article
Energy & Fuels
Ali Ihsan Karayigit, Nevin Azeri, Riza Gorkem Oskay, James C. Hower
Summary: This study investigated the mineralogical and elemental compositions of three sampling profiles from different sectors of the Cayırhan coalfield. The most significant difference between the Tv and Tb splits was found to be in the mineralogical composition. The presence of zeolite minerals and carbonate minerals in the Tv and Tb splits of the BA and BB profiles suggests favorable alkaline conditions for natural zeolite formation. In contrast, the presence of zeolite minerals and authigenic K-feldspar grains in the BC profile implies a semi-open hydrogeological system for transferring necessary ions for zeolite formation.
INTERNATIONAL JOURNAL OF COAL GEOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Long Sun, Hong-Yan Zhang, Fu-Qiang Zhang, Li Wang, Xian-Ming Zhang
Summary: This study investigates the structural evolution and assembly of clusters through inter-cluster transformation, which is crucial for understanding crystal growth and accurate synthesis of cluster-based materials. The researchers demonstrate diverse transformation products by tuning synthetic parameters and amine composition using a ligand-free T3-InS cluster as the precursor. The role of amine in the transformation processes and the competition between amines and cluster-derived intermediates are examined and a S(N)1-like mechanism for surface reaction is proposed. The study provides insights into the role of amines in nucleation processes and a novel method for accurate synthesis of cluster-based materials with specific Tn skeletons.
MATERIALS CHEMISTRY FRONTIERS
(2022)
Article
Engineering, Environmental
Huijuan Liu, Keyan Wei, Chao Long
Summary: In this study, core-shell composites of NaY zeolite coated with mesoporous SiO2 were synthesized to improve the hydrophobicity and mass diffusion of the zeolite. The results showed that the composites exhibited enhanced adsorption capacity and diffusion of volatile organic compounds (VOCs). The coating of NaY zeolite with mesoporous SiO2 promoted the diffusion of VOCs into the composites, and the NaY@meso-SiO2-1.2 composite showed the strongest adsorption ability and excellent hydrophobicity at RH = 50%.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Ying-Chieh Hung, Chieh-Ming Hsieh, Hiroshi Machida, Shiang-Tai Lin, Yusuke Shimoyama
Summary: A hybrid modeling approach combining the COSMO-SAC model with classical molecular dynamics was proposed to study the phase behavior of systems containing alkylene glycol derivatives, showing that conformational populations significantly influence the accuracy in predicting liquid-liquid equilibrium.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Review
Chemistry, Applied
Bin Yue, Shanshan Liu, Yuchao Chai, Guangjun Wu, Naijia Guan, Landong Li
Summary: Material-based emerging separation techniques, such as zeolite membrane separation and adsorptive separation, have gained attention as alternatives to traditional methods. Zeolites, with their structure characteristics, have been successfully utilized in important separation processes as versatile sieves and adsorbents. This article discusses the synthesis strategies for zeolite membranes and emphasizes uniformly-oriented membranes. It also summarizes industrial and popular adsorptive separations using zeolite adsorbents.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Salvador R. G. Balestra, Bruno Martinez-Haya, Norge Cruz-Hernandez, Dewi W. Lewis, Scott M. Woodley, Rocio Semino, Guillaume Maurin, A. Rabdel Ruiz-Salvador, Said Hamad
Summary: We studied the nucleation of Zeolitic Imidazolate Frameworks using computational techniques. The ZnIm(4) cluster was found to be the prevalent cluster in the pre-nucleating solution. However, other clusters such as ZnIm(3), Zn(2)Im(7), Zn(3)Im(9), Zn(3)Im(10), or Zn(4)Im(12) also exist in appreciable quantities. We observed that glassy clusters are the first to form in the nucleation process, which then undergo transformation to crystal structures.
Article
Engineering, Chemical
Mariana C. N. Bessa, Azahara Luna-Triguero, Jose M. Vicent-Luna, Paulo M. O. C. Carmo, Mihalis N. Tsampas, Ana Mafalda Ribeiro, Aliirio E. Rodrigues, Sofia Calero, Alexandre F. P. Ferreira
Summary: Two industrial dual-step pressure swing adsorption (PSA) processes were designed and simulated to obtain high-purity methane, CO2, and syngas from a gas effluent of a CO2 electroreduction reactor using different design configurations. NaX and MFI zeolites were selected from the investigated set for simulation. Case study 1 achieved 90.5% methane purity with a 95.2% recovery, whereas case study 2 obtained methane with a 97.5% purity and 95.3% recovery. Both case studies produced high-purity CO2 (>97%) and syngas with a H-2/CO ratio above 4. However, case study 2 had a significantly higher energy consumption compared to case study 1 (64.9 vs 29.8 W h mol(CH4) (-1)).
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Gabriela Jajko, Juan Jose Gutierrez Sevillano, Sofia Calero, Waclaw Makowski, Pawel Kozyra
Summary: This study investigated the adsorption of toluene in UiO-66 materials. Toluene is a volatile, aromatic organic molecule that is recognized as the main component of VOCs. The UiO-66 material was found to successfully capture toluene through adjustments to the force field parameters and analysis of occupation profiles and radial distribution functions. These findings provide an understanding of the mechanism of toluene adsorption on UiO-66.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Xiucheng Huang, Ana Martin-Calvo, Martijn J. J. Mulder, Sjoerd C. J. van Acht, Juan Jose Gutierrez-Sevillano, Julio C. Garcia-Navarro, Sofia Calero
Summary: This study focuses on the performance of zeolitic imidazolate frameworks (ZIFs) for hydrogen purification from coke oven gases (COG). Molecular simulation is used to compare different ZIF topologies and analyze the separation performance. The findings reveal that ZIFs with smaller pore sizes exhibit better separation of hydrogen from carbon monoxide and nonpolar molecules. The adsorption of carbon dioxide is strongly influenced by the structure's polarizability, while the adsorption of other components depends on their pore sizes. The study provides valuable information for selecting high-performance ZIFs for hydrogen purification.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Computer Science, Artificial Intelligence
Luis M. Antunes, Keith T. Butler, Ricardo Grau-Crespo
Summary: Models constructed with machine learning techniques can be used to scan the space of inorganic materials and predict the thermoelectric behavior of novel materials with lower computational cost and good performance, providing a new method for the design of new thermoelectric materials.
MACHINE LEARNING-SCIENCE AND TECHNOLOGY
(2023)
Article
Nanoscience & Nanotechnology
Jose Luis Nunez-Rico, Juanjo Cabezas-Gimenez, Vanesa Lillo, Salvador R. G. Balestra, Jose Ramoon Galan-Mascaros, Sofia Calero, Anton Vidal-Ferran
Summary: Metal-organic frameworks (MOFs) with tunable properties and controlled dimensionality have shown promising potential for various applications. The incorporation of chirality into MOFs opens up new strategies for chiral separation, which is crucial in the pharmaceutical industry. In this study, computational modeling and experiments were combined to demonstrate the efficiency, versatility, robustness, and reusability of TAMOF-1-packed HPLC columns as the chiral stationary phase. The in silico studies predicted plausible separations of chiral compounds from different families, and the experimental results confirmed the validity of the models and the high performance of TAMOF-1 columns. The use of in silico screening in chiral chromatography is an unprecedented achievement.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Environmental
Dominika O. Wasik, Ana Martin-Calvo, Juan Jose Gutierrez-Sevillano, David Dubbeldam, Thijs J. H. Vlugt, Sofia Calero
Summary: Formic acid production from CO2 can reduce carbon dioxide emissions while synthesizing a versatile product. This study investigated the confinement effects of metal-organic frameworks on CO2 hydrogenation to formic acid through molecular simulations. The results showed that metal-organic frameworks, such as UiO-66, can enhance the production of formic acid by shifting the thermodynamic equilibrium.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Pablo Romero-Marimon, Juan Jose Gutierrez-Sevillano, Sofia Calero
Summary: We examined the impact of aluminum distribution on CO2 adsorption properties in MFI, MOR, and ITW zeolites. Through molecular simulations, we found that CO2 adsorption in MFI is determined by the number rather than the distribution of aluminum atoms. In MOR, the distribution of aluminum in the C-channel plays a crucial role in heat adsorption. ITW zeolite, with its small-pore structure, showed high heat adsorption values only at low aluminum concentrations.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Miguel A. Urbiztondo Castro, Sergio G. Rodrigo, Said Hamad
Summary: This study utilizes deep learning to predict energy values on a catalyst surface and achieves a significant reduction in computational time. The research overcomes the limitations of traditional methods and has the potential to revolutionize efficiency in the chemical industry.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Jose J. Plata, Ernesto J. Blancas, Antonio M. Marquez, Victor Posligua, Javier Fdez Sanz, Ricardo Grau-Crespo
Summary: Nanostructuring is an effective approach to improve the thermoelectric behavior of materials. However, the effectiveness is limited if excessively small particle sizes are necessary to decrease the lattice thermal conductivity. This study combines ab initio calculations and machine learning to systematically investigate the thermoelectric properties of nanostructured AgInTe2, showing that ZT values up to 2 can be achieved at 700 K with an average grain size in the range of 10-100 nm.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Shivani Grover, Stefan Burger, Keith T. Butler, Karina Hemmer, Pia Vervoorts, Gregor Kieslich, Ricardo Grau-Crespo
Summary: ABX(3) molecular perovskites are receiving attention in the field of ferroelectrics and barocalorics, as their mechanical properties play an important role. The modular building principle of perovskite motif allows systematic studies on the interplay of composition, structure, and properties. In this study, the impact of M2+ metal species on the mechanical properties of [(nPr)(3)(CH3)N]M(C2N3)(3) molecular perovskite series was investigated through lattice dynamic calculations and high-pressure powder X-ray diffraction. The relationship between geometric factors and mechanical properties, evaluated using bulk modulus, agrees with chemical intuition. These results contribute to the better understanding and design of materials with targeted macroscopic properties.
Article
Chemistry, Multidisciplinary
Mike Pols, Victor Brouwers, Sofia Calero, Shuxia Tao
Summary: Machine-learned force fields, trained with an active learning scheme against accurate density functional theory calculations, allow us to investigate defect migration in halide perovskites. We find that halide interstitials migrate faster than halide vacancies, with interstitials having shorter migration paths. Both types of defects migrate faster in CsPbI3 than in CsPbBr3, attributed to the less compact packing of ions in CsPbI3 leading to more frequent defect migration jumps.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Vasileios Fotopoulos, Ricardo Grau-Crespo, Alexander L. Shluger
Summary: Using DFT calculations and grand canonical thermodynamic analysis, we determined the equilibrium molar fractions of copper vacancies (V-Cu), hydrogen interstitials (H-i), and their complexes in bulk Cu over a wide range of temperature and hydrogen pressure values. Our results demonstrate that the molar fractions of both V-Cu and H-i are generally low, consistent with experimental data. The formation of H-i-V-Cu complexes has lower energy compared to isolated defects; however, the presence of hydrogen has a minimal impact on the increase in vacancy molar fraction at hydrogen pressures below 100 bar. Only at relatively high hydrogen pressures (>10 kbar) in the presence of Cu vacancies, the molar fraction of hydrogen reaches the same order of magnitude as that of vacancies. These findings impose thermodynamic limits on hydrogen-induced vacancy clustering and void formation in bulk Cu.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)