Article
Chemistry, Physical
Michiko Atsumi, Jia-Jia Zheng, Erik Tellgren, Shigeyoshi Sakaki, Trygve Helgaker
Summary: This study investigated the adsorption of CO2, acetone, and methanol on UiO-66 using DFT and post-Hartree-Fock calculations. The results showed that UiO-66 can adsorb multiple molecules, and the adsorption capacity and binding energy depend on the type of molecule and adsorption site. NMR spectra were also used to study the adsorption of CO2 on UiO-66.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Dayton J. Vogel, Jessica M. Rimsza, Tina M. Nenoff
Summary: Reactive gas formation in pores of metal-organic frameworks (MOFs) is known to cause framework destruction, understanding these mechanisms are key to future durability design. This study used AIMD simulations for the first time to predict competitive adsorption of mixed acid gases in RE-DOBDC MOFs and identified spontaneous formation of HONO as a result of deprotonation of the MOF organic linker. This study provides a novel mechanism for HONO formation in MOFs and offers a methodology for predicting future gas interactions in new nanoporous materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Marcin Rybicki, Joachim Sauer
Summary: An anharmonic approach for molecule-surface vibrations using rigid body coordinates is presented, and its application to the adsorption of methane on zeolite and metal-organic frameworks is described. The coupling between intrasystem vibrations and molecule-surface vibrations is also considered. The calculated results show good agreement with experimental values within the chemical accuracy range.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Xinyao Liu, Kent O. Kirlikovali, Zhijie Chen, Kaikai Ma, Karam B. Idrees, Ran Cao, Xuan Zhang, Timur Islamoglu, Yunling Liu, Omar K. Farha
Summary: A study highlighted a method to synthesize MOF-808 in water, producing products with high crystallinities and porosities, and allowing straightforward tuning of pore environment. By modifying the modulator used, it is possible to adjust the water adsorption properties of MOF-808 and its solid-state catalytic performance.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Physical
Bo Han, Anutosh Chakraborty
Summary: This study focuses on using Grand Canonical Monte Carlo simulation to investigate the water adsorption behavior of functionalized MOFs. The simulation results were compared with experimental data, showing the accuracy of the simulation. The findings demonstrate the potential of GCMC simulation in designing and optimizing MOFs for heat transformation applications.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Applied
Yan-Hua Fan, Ya-Xin Li, Wen-Jie Zhu, Yan Bai, Dong-Bin Dang
Summary: In this study, the adsorption performances of four 3D polyoxometalate-based metal-organic frameworks (POMOFs) on organic dyes were systematically studied. The results showed that these compounds exhibited highly sensitive selective adsorption behavior towards the cationic dye methylene blue. The study provides a new idea for the adsorption and separation of cationic dyes in wastewater by constructing materials with a large amount of charge on the surface.
Article
Multidisciplinary Sciences
Yan Su, Ken-ichi Otake, Jia-Jia Zheng, Satoshi Horike, Susumu Kitagawa, Cheng Gu
Summary: Efficient separation of water isotopologues at room temperature has been achieved by constructing porous coordination polymers with flip-flop molecular motions to regulate the diffusion rates of water isotopologues. This method shows promise for high-performance vapor separation.
Article
Biochemistry & Molecular Biology
Liliana Giraldo, Fernando Gomez-Granados, Juan Carlos Moreno-Pirajan
Summary: This research immobilizes CALB on MOF-199 and ZIF-8 and uses them in the transesterification reaction for biodiesel production. The highest adsorption capacity of 26.9 mg•g-1 Lipase is achieved using ZIF-8 at 45°C and an initial protein concentration of 1.20 mg•mL-1. CALB is physically adsorbed on ZIF-8 and chemically adsorbed on MOF-199. Kinetic studies show that the adsorption kinetics follow the Elovich model for both biocatalysts.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Primoz Poredos, He Shan, Chenxi Wang, Fangfang Deng, Ruzhu Wang
Summary: Sorption and radiative sky cooling technologies have the potential to provide decentralized fresh water, but continuous operational devices are needed. Current energy materials and system designs have limitations that hinder continuous AWH. By addressing these challenges, 24-hour continuous fresh water generation can be achieved.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Thermodynamics
Tahmid Hasan Rupam, Farhana Jesmin Tuli, Israt Jahan, Mujib L. Palash, Anutosh Chakraborty, Bidyut Baran Saha
Summary: MOFs, a new type of porous coordination polymers, have attracted the interest of researchers worldwide. In this study, water adsorption isotherms onto three different MOFs were obtained and their performance in adsorption heat pumps was evaluated. Results showed that the studied MOFs exhibited excellent performance in water-based adsorption cooling systems.
THERMAL SCIENCE AND ENGINEERING PROGRESS
(2022)
Article
Materials Science, Multidisciplinary
Harpreet Singh, Anuj Goyal, Sanjeev K. Bhardwaj, Madhu Khatri, Neha Bhardwaj
Summary: This study investigated the use of metal-organic framework derived beads for the removal of tartrazine from aqueous solutions through batch adsorption experiments. The UiO-66 MOF was synthesized and transformed into highly robust millimeter-sized beads. The adsorption process was influenced by parameters such as initial pH, adsorption time, initial tartrazine concentration, and temperature. The results showed a high removal efficiency of 97% at an optimum pH of 2.0 and a contact time of 120 minutes. The adsorption followed the pseudo-second-order model, and the Langmuir model was found to be the most suitable for describing the adsorption of dye on the beads. The adsorbent demonstrated good regeneration capability, with no significant loss in adsorption capacity for at least five cycles.
MATERIALS SCIENCE AND ENGINEERING B-ADVANCED FUNCTIONAL SOLID-STATE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Adrian Fuchs, Fabian Knechtel, Haoze Wang, Zhe Ji, Stefan Wuttke, Omar M. Yaghi, Evelyn Ploetz
Summary: Metal-organic frameworks (MOFs) are porous materials that can easily absorb and release water, making them ideal for atmospheric water harvesting applications. In this study, a new method using Raman spectroscopy was used to investigate the behavior of MOF-801 at the single-crystal level, providing valuable insights into its water adsorption capabilities. The results revealed significant differences in water uptake between the single-crystal and bulk material.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xiaoqian Zhu, Tian Ke, Jingyi Zhou, Yifei Song, Qianqian Xu, Zhiguo Zhang, Zongbi Bao, Yiwen Yang, Qilong Ren, Qiwei Yang
Summary: Developing adsorbents with multiple merits in capacity, selectivity, mass transfer, and stability is crucial for producing high-purity C2H2 for advanced polymers and the electronic industry. We demonstrate a vertex strategy to create adsorbents with these merits through rationally designing the vertex groups of a wavy-shaped framework in 2D metal-organic frameworks.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Arijit Halder, Ryan A. Klein, Sarah Shulda, Gavin A. McCarver, Philip A. Parilla, Hiroyasu Furukawa, Craig M. Brown, C. Michael McGuirk
Summary: Step-shaped adsorption-desorption of gaseous payloads by flexible metal-organic frameworks can facilitate the delivery of large usable capacities with reduced energetic penalties. The multivariate linker approach is a powerful tool for tuning the phase change behavior of flexible frameworks. In this work, a multivariate framework was developed with a considerably reduced threshold pressure and desirable adsorption-desorption profile for efficient storage and delivery of weakly physisorbing species.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Kalpita Mudoi, Rinki Brahma, Jubaraj Bikash Baruah
Summary: The study reveals the interaction ability of a secondary building unit (SBU) and its corresponding coordination polymer with ionic dyes, showing oscillation concentration of the adsorbed dye. The pH change caused by ion exchange guides the adsorption at a particular time.
INORGANIC CHEMISTRY COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Fortuna Ponte, GiovanniMaria Piccini, Emilia Sicilia, Michele Parrinello
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2020)
Article
Chemistry, Multidisciplinary
Severin Merget, Lorenzo Catti, GiovanniMaria Piccini, Konrad Tiefenbacher
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Multidisciplinary
Melina Knezevic, Michael Heilmann, Giovanni Maria Piccini, Konrad Tiefenbacher
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Physical
Emanuele Grifoni, GiovanniMaria Piccini, Michele Parrinello
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2020)
Article
Multidisciplinary Sciences
Emanuele Grifoni, GiovanniMaria Piccini, Johannes A. Lercher, Vassiliki-Alexandra Glezakou, Roger Rousseau, Michele Parrinello
Summary: The study investigates the gradual transition of BrOnsted acid sites in different pore size zeolites to hydronium ions using ab initio molecular dynamics and enhanced sampling techniques. It is found that the concentration of water molecules significantly affects the standard free energy of formed complexes, while entropy increases linearly with water concentration in pores, favoring proton solvation.
NATURE COMMUNICATIONS
(2021)
Article
Multidisciplinary Sciences
Luigi Bonati, GiovanniMaria Piccini, Michele Parrinello
Summary: The development of enhanced sampling methods has expanded the scope of atomistic simulations, allowing the study of long-time phenomena with accessible computational resources. By identifying appropriate collective variables and utilizing machine learning and probability-enhanced sampling techniques, efficient transfer operator eigenfunctions can be extracted to accelerate the sampling of rare events, demonstrating the versatility and power of this approach across various systems.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Review
Chemistry, Physical
GiovanniMaria Piccini, Mal-Soon Lee, Simuck F. Yuk, Difan Zhang, Greg Collinge, Loukas Kollias, Manh-Thuong Nguyen, Vassiliki-Alexandra Glezakou, Roger Rousseau
Summary: Ab initio molecular dynamics simulations combined with enhanced sampling techniques are becoming widespread methods to investigate chemical phenomena in catalytic systems. These methods automatically consider finite temperature effects, anharmonicity, and collective dynamics, which significantly affect reaction free energy landscapes. In contrast, standard ab initio static approaches rely on coarse-grained descriptions of reaction potential energy surfaces to assess reaction free energies. Enhanced sampling ab initio molecular dynamics allows for first principles simulations of increasingly complex systems, such as solid/liquid catalytic interfaces.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Marcin Rybicki, Kaido Sillar, Joachim Sauer
Summary: This study employs quantum chemical calculations combined with molecular statistics to calculate the enthalpies and Gibbs free energies of CH4 adsorption at Bronsted acid sites and silica wall sites in zeolites. The results show that zeolites with different Si/Al ratios have different adsorption isotherms, and the calculated results agree well with experimental results.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Kaido Sillar, Ivar Koppel
Summary: In this study, quantum chemistry and molecular statistics are used to calculate the Gibbs free energies, enthalpies, and entropies of carbon dioxide adsorption on open metal sites in the metal-organic framework Mg-2(dobdc), also known as CPO-27-Mg and Mg-MOF-74. Gas-surface interaction energies are calculated using periodic MP2 and DFT+D methods for the crystal framework and CCSD(T) for the adsorption site. Thermodynamic functions are obtained from anharmonic vibrational frequencies for isolated sites and for CO2 molecules interacting with neighboring molecules at higher surface coverages. Including lateral adsorbate-adsorbate interactions improves the agreement between experimental isotherms and ab initio calculations of thermodynamic functions to within +/- 1 kJ/mol.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Kaido Sillar, Arpan Kundu, Joachim Sauer
Summary: In this study, grand canonical Monte Carlo simulations were performed to predict adsorption selectivities for three binary mixtures in the metal-organic framework Mg-2(dobdc). Based on the simulations, the performance of IAST was evaluated in conditions where nonideal adsorbed phase occurs. The results showed that IAST underestimated the selectivities compared to the simulation results, indicating that the real material can be a better adsorbent for gas separation.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Organic
Michael Heilmann, Melina Knezevic, GiovanniMaria Piccini, Konrad Tiefenbacher
Summary: A modular synthetic platform for constructing flexible glycoluril-derived molecular tweezers was developed and investigated for their binding properties towards 16 organic amines through H-1 NMR titration. The results demonstrated that certain structural modifications can lead to potent and selective binding of natural polyamines by the molecular tweezers.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Arpan Kundu, Kaido Sillar, Joachim Sauer
Article
Chemistry, Physical
Martina Danese, Marta Bon, GiovanniMaria Piccini, Daniele Passerone
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2019)
Article
Chemistry, Physical
Florian R. Rehak, Giovannimaria Piccini, Maristella Alessio, Joachim Sauer
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2020)