Article
Biochemistry & Molecular Biology
Marhaina Ismail, Mohamad Azmi Bustam, Nor Ernie Fatriyah Kari, Yin Fong Yeong
Summary: Ideal Adsorbed Solution Theory (IAST) is a predictive model that can predict multicomponent adsorption equilibrium and selectivity based on experimental single-component adsorption isotherms. In this study, IAST calculations were used to predict the mixed gas adsorption isotherms of CO2 and CH4 using the Python package (pyIAST). The results showed that CO2 adsorption was more favorable and had a higher adsorbed amount compared to CH4 adsorption, indicating that Mg-gallate can be a potential adsorbent for the separation of CO2/CH4 mixed gas.
Article
Chemistry, Physical
Chunli Xu, Zhifeng Yang, Lei Shi, Yu Yin, Min Lu, Mengxuan Liu, Aihua Yuan, Hong Wu, Xiao-Ming Ren, Shaobin Wang, Hongqi Sun
Summary: Adsorbents based on CuI for p-complexative separation of C2H4/C2H6 have attracted widespread interests. However, challenges remain in terms of low separation efficiency and poor stability. In this study, a novel CuCoM-DS adsorbent with superior performance in C2H4/C2H6 separation was successfully synthesized by encapsulating active Cu and auxiliary Co species within the nanopores of MIL-101 using a double-solvent method. The best sample 1.5CuCoM-DS exhibited high C2H4 adsorption capacity and selectivity, maintaining over 90% of fresh C2H4 uptake after exposure to air for 12 days.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Chemistry, Physical
Miao Chang, Tongan Yan, Yan Wei, Jie-Xin Wang, Dahuan Liu, Jian-Feng Chen
Summary: By utilizing a single-molecule SF6 trap in a metal-organic framework, efficient SF6 recovery and separation have been achieved. This trap exhibits unprecedented selectivity and adsorption capacity, making it an ideal adsorbent.
CHEMISTRY OF MATERIALS
(2022)
Article
Environmental Sciences
Dong-Ik Song, Jiyeon Choi, Won Sik Shin
Summary: The article presents a slightly modified version of the Song isotherm model, the Modified Song Model (MSM), which allows for more efficient and accurate calculation of the Ideal Adsorbed Solution Theory (IAST). The MSM was shown to satisfy different adsorption models at varying concentrations and provided approximate parameter estimation methods. Additionally, the article discusses the application of MSM in single-solute sorption studies and its advantages over other three-parameter models.
ENVIRONMENTAL TECHNOLOGY
(2021)
Article
Engineering, Chemical
Yue Wu, Shanshan Wang, Wenxiang Zhang, Shuhui Chen, Zhonghui Zhang, Bolun Yang, Shengping Li, Heping Ma
Summary: The study demonstrates the effectiveness of a microporous metal-organic framework (SBMOF-1) in trapping F-gases and its potential for capturing F-gases from semiconductor etching exhaust.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Engineering, Chemical
Hao Su, Shuainan Ni, Chenhao Liu, Xiaoqi Sun
Summary: In this study, four fatty acid-based ionic liquids were synthesized to remove aluminum impurities in ion-adsorption rare earth ores. One specific ionic liquid, [methyltrioctylammonium][neodecanoate], showed better extraction and separation performance for aluminum. A process combining fractional extraction and extraction-precipitation was developed to remove impurity ions in the leaching solution of magnesium sulfate and achieve high concentration rare earth chloride product with high purity.
MINERALS ENGINEERING
(2023)
Article
Nanoscience & Nanotechnology
Wenxiang Zhang, Yinhui Li, Yue Wu, Wenbo Huang, Shanshan Wang, Yu Fu, Wuju Ma, Xiaoyu Li, Heping Ma
Summary: A polypyrene porous organic framework (Ppy-POF) with an extended pi-conjugated structure and excellent acid resistance was constructed. It demonstrated exceptional adsorption selectivity for highly polarizable F-gases and xenon (Xe) due to the abundant pi-conjugated structures and gradient electric field distribution. The selective adsorption was attributed to the strong charge-transfer effect and polarization effect between Ppy-POF and the gases.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Shu-Li Yao, Hui Xu, Teng-Fei Zheng, Sui-Jun Liu, Jing-Lin Chen, He-Rui Wen
Summary: A 3D metal-organic framework with 8-connected bcg topology was synthesized and found to selectively detect methylamine, showing good thermal and chemical stability.
CRYSTAL GROWTH & DESIGN
(2021)
Article
Chemistry, Inorganic & Nuclear
Gregory S. Day, Gerard T. Rowe, Carlos Ybanez, Ray O. Ozdemir, Jason Ornstein
Summary: One major challenge for long-term human space exploration is the need for a breathable atmosphere. Researchers have found that metal-organic frameworks have the ability to adsorb acetylene, which is crucial for removing toxic substances in the byproduct stream during CO2 reduction.
INORGANIC CHEMISTRY
(2022)
Article
Environmental Sciences
Liqing Li, Chenhao Liu, Hepeng Zhang, Bin Huang, Bing Luo, Chao Bie, Xiaoqi Sun
Summary: This study successfully achieved impurities removal and enrichment of rare earth elements in ion-adsorbed type rare earth ore by using specific materials. The method reduces the loss rate of rare earth elements and improves product purity, while also benefiting environmental protection and resource recycling.
JOURNAL OF ENVIRONMENTAL MANAGEMENT
(2022)
Article
Engineering, Chemical
Farhad Gharagheizi, David S. Sholl
Summary: This paper systematically evaluates the accuracy of the ideal adsorbed solution theory (IAST) for gas adsorption using a large collection of binary experimental data, which will be valuable for future efforts to test or develop mixing theories that improve upon FAST. This analysis includes data from 63 gas mixtures of 37 different molecular species and 174 different adsorbents, making it the most systematic evaluation to date of the accuracy of IAST for gas adsorption.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Review
Chemistry, Multidisciplinary
Shan-Qing Yang, Tong-Liang Hu, Banglin Chen
Summary: The release of anthropogenic greenhouse gases poses a global threat and the efficient capture and separation of these gases is of great significance. Metal-organic framework (MOF) materials, with their unique structure and high surface areas, have been extensively studied for their applicability in this field. This review provides a comprehensive account of the progress in using MOFs as adsorbents for capture and separation of greenhouse gases, including carbon dioxide, methane, nitrous oxide, and fluorocompounds. The strategies, performance, mechanisms, challenges, and perspectives associated with the development of MOF materials are discussed.
SCIENCE CHINA-CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Hudson A. Bicalho, P. Rafael Donnarumma, Victor Quezada-Novoa, Hatem M. Titi, Ashlee J. Howarth
Summary: In this study, post-synthetic modification of a rare-earth cluster-based MOF was achieved through transmetalation, with reproducible results observed. The transmetalated materials were fully characterized and compared to the parent MOF, showing successful metal exchange in the nonanuclear cluster nodes.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Yan Li, Hongwei Chen, Chaoran Wang, Yu Ye, Libo Li, Xiaowei Song, Jihong Yu
Summary: This study synthesized SAPO-35 zeolites with various silicon contents and modulated acidities and polarities by using a specific template under hydrothermal conditions. The results showed that the silicon content in the framework is essential for regulating the CO2 adsorption performance, and increasing Bronsted acidity can significantly enhance the selectivity of CO2 over N-2.
Article
Chemistry, Physical
Elliott L. Bruce, Veselina M. Georgieva, Maarten C. Verbraeken, Claire A. Murray, Ming-Feng Hsieh, William J. Casteel, Alessandro Turrina, Stefano Brandani, Paul A. Wright
Summary: Small pore zeolites like merlinoite have high potential for selective CO2 adsorption. Na- and Cs-exchanged forms shift to narrow-pore form after dehydration, while K-form remains wide-pore. K- and Cs-forms show effects of CO2 adsorption on cation site distributions and framework configuration.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Eunja Kim, Philippe F. Weck, Jeffery A. Greathouse, Margaret E. Gordon, Charles R. Bryan
CHEMICAL PHYSICS LETTERS
(2020)
Article
Chemistry, Physical
Hasini S. Senanayake, Jeffery A. Greathouse, Anastasia G. Ilgen, Ward H. Thompson
Summary: Water in nano-scale confining environments plays a crucial role in various biological, material, and geological systems, leading to significant changes in its structure and dynamics. Vibrational spectroscopy has emerged as a powerful tool for studying these alterations, with a focus on understanding the connection between spectroscopic features and molecular-level details. Molecular dynamics simulations were used in this study to investigate the linear infrared and Raman spectra of isotopically dilute HOD in D2O confined in hydroxylated amorphous silica slit pores. The confinement effect primarily results in a blueshift in the frequency of OH groups donating a hydrogen bond to the silica surface, showcasing the weaker hydrogen-bond accepting properties of silica oxygens compared to water molecules.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Biochemistry & Molecular Biology
Calen J. Leverant, Chad W. Priest, Jeffery A. Greathouse, Mark K. Kinnan, Susan B. Rempe
Summary: Lithium nitride has been proposed as a neutralization reagent for chemical warfare agents due to its ability to produce nucleophilic ammonia molecules and hydroxide ions. Quantum chemical calculations have provided insight into the neutralization process of Li3N, particularly in relation to the CWA VX. Experimental validation has confirmed the results obtained from the calculations.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Review
Chemistry, Physical
Randall T. Cygan, Jeffery A. Greathouse, Andrey G. Kalinichev
Summary: Clayff, a general-purpose force field for molecular simulations of layered materials and fluid interfaces, is widely used in atomistic computational modeling for predicting properties of various materials due to its success, transferability, and simple functional form. Recent modifications have extended its applications to surface terminations, providing potential for future developments.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Joshua P. Allers, Chad W. Priest, Jeffery A. Greathouse, Todd M. Alam
Summary: The ability to predict transport properties of liquids using machine learning methods shows promising results in accurately forecasting diffusion properties of pure liquids. Artificial Neural Networks have been effectively used in this study to model diffusion of pure liquids, aiding in the design of materials and processes for various applications.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Physical
Calen J. Leverant, Jacob A. Harvey, Todd M. Alam, Jeffery A. Greathouse
Summary: Predicting the diffusion coefficient of fluids under nanoconfinement is crucial for various applications, and a machine learning model trained on a subset of MD data showed good predictive ability for Lennard-Jones fluids in pores. By using MD simulations and an artificial neural network model, the study presented a new approach for predicting fluid diffusion coefficients.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Geochemistry & Geophysics
Daniel M. Long, Jeffery A. Greathouse, Guangping Xu, Katherine L. Jungjohann
Summary: This study investigated the structural properties of the anionic surfactant dioctyl sodium sulfosuccinate (AOT) adsorbed on the mica surface using molecular dynamics simulation. The simulations revealed that the adsorption mechanism depended on the surface loading and the presence of monovalent and divalent cations. At low loading, cylindrical micelles formed on the surface, while at high loading, adsorbed bilayers were observed. Experimental confirmation of the adsorbed micelle structure was obtained with cryogenic electronic microscopy.
Article
Chemistry, Physical
Hasini S. Senanayake, Jeffery A. Greathouse, Ward H. Thompson
Summary: The structural and dynamical properties of nanoconfined solutions differ from those of bulk systems, and understanding these changes is important for controlling synthetic nanostructured materials. The effects of confinement on nanoscale electrolyte solutions were studied using molecular dynamics simulations. It was found that linear infrared spectroscopy has limitations as a probe of confined water, while the reorientational and spectral diffusion dynamics of OH are significantly slowed by confinement.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Kevin Leung, Jeffery A. Greathouse
Summary: This study used ab initio molecular dynamics calculations to investigate the coordination structure and free energy changes of Cu(II) cation dimers on silica surfaces, revealing a stronger tendency for Cu(II) dimerization on silica surfaces. Understanding the adsorption processes of metal cations on mineral surfaces is crucial for environmental cleanup efforts and toxic waste retention.
COMMUNICATIONS CHEMISTRY
(2022)
Review
Chemistry, Physical
Anastasia G. Ilgen, Kevin Leung, Louise J. Criscenti, Jeffery A. Greathouse
Summary: Reactions at solid-water interfaces are crucial in water treatment systems, catalysis, and chemical separations. Nanoconfinement can significantly alter the interfacial reactivity of a solid surface, which traditional measurements and models fail to capture. This review summarizes recent advances in experimental and theoretical studies, focusing on the adsorption process at solid-water interfaces under nanoconfinement.
ANNUAL REVIEW OF PHYSICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Jeffery A. Greathouse, Matthew J. Paul, Guangping Xu, Matthew D. Powell
Summary: Strong gas-mineral interactions and slow adsorption kinetics affect gas mobility in zeolite pores, especially at pore-limiting window sites. This study combines molecular simulations and experiments to investigate noble gas adsorption and mobility in two zeolites. The results show that even the largest gas (Rn) can be accommodated in both zeolites, but gas mobility is significantly hindered in clinoptilolite. The experimental results confirm the presence of a kinetic barrier to Xe uptake, resulting in reverse Kr/Xe selectivity. A kinetic model is used to compare gas diffusivity in the zeolite pores.
CLAYS AND CLAY MINERALS
(2023)
Article
Chemistry, Physical
Calen J. Leverant, Jeffery A. Greathouse, Jacob A. Harvey, Todd M. Alam
Summary: Predicting diffusion in confined environments is possible using empirical expressions and machine learning models. This research applies artificial neural network (ANN) models to predict the self-diffusion coefficients of real liquids in both bulk and pore environments. The results show excellent agreement between simulated and experimental diffusion coefficients, and the ANN models accurately reproduce the diffusion data for both bulk and confined liquids.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Hasini S. S. Senanayake, Pubudu N. N. Wimalasiri, Sahan M. M. Godahewa, Ward H. H. Thompson, Jeffery A. A. Greathouse
Summary: We propose a classical interatomic force field, silica-DDEC, for describing the interactions between amorphous and crystalline silica surfaces. The model is parameterized using density functional theory-based charges. Charges for silica surfaces are determined using the density-derived electrostatic and chemical (DDEC) method, which accurately reproduces atomic charges and electrostatic potential away from the atom sites. Lennard-Jones parameters are determined to accurately describe the density, coordination defects, local coordination geometry, and water-silica interatomic distances. The resulting model provides a general description of fully flexible amorphous and crystalline silica surfaces and their interactions with liquids of varying structure and protonation state.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
N. Scott Bobbitt, Joshua P. Allers, Jacob A. Harvey, Derrick Poe, Jordyn D. Wemhoner, Jane Keth, Jeffery A. Greathouse
Summary: Ionic liquids have complex behavior, making it difficult to predict their properties, especially in confined environments. We have developed machine learning models based on molecular dynamics simulations to predict diffusion and conductivity of ionic liquids across a wide temperature range. These models use simple physical descriptors of the ions and can provide accurate results with minimal computational effort by using SMILES codes.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Jeffery A. Greathouse, Tyler J. Duncan, Anastasia G. Ilgen, Jacob A. Harvey, Louise J. Criscenti, Andrew W. Knight
Summary: In this study, a combined MD simulation and XAFS spectroscopic investigation was conducted to explore the adsorption mechanism of aqueous iron on nanoconfined amorphous silica surfaces. The simulation results demonstrated a significant dependence of iron adsorption on silica surface charge and a notable effect of pore size on the adsorption of Fe(ii). Adsorption trends varied with concentration and aqueous Fe speciation, and the coordination environment of adsorbed iron was found to vary significantly with the type of anion present.
ENVIRONMENTAL SCIENCE-NANO
(2021)