Article
Multidisciplinary Sciences
Heng Zeng, Mo Xie, Ting Wang, Rong-Jia Wei, Xiao-Jing Xie, Yifang Zhao, Weigang Lu, Dan Li
Summary: Metal-organic frameworks (MOFs) are known for their precise control of structures and functions on a molecular level, but designing local flexibility in the MOF framework for dynamic molecular sieving remains challenging. A newly reported MOF material, JNU-3a, features one-dimension channels with embedded molecular pockets that can selectively adsorb propylene and propane under different pressures, showcasing the potential of dynamic molecular sieving.
Review
Chemistry, Multidisciplinary
Muruganantham Rethinasabapathy, Seyed Majid Ghoreishian, Seung-Kyu Hwang, Young-Kyu Han, Changhyun Roh, Yun Suk Huh
Summary: This review discusses recent progress and main research trends in hydrogen isotope storage and separation, with a focus on tritium. It highlights the use of metal hydrides, nanoporous zeolites, metal organic frameworks (MOFs), and 2-D layered graphene, h-BN, and MXenes based on their diverse functionalities.
ADVANCED MATERIALS
(2023)
Article
Engineering, Chemical
Nicholas C. Means, Daniel J. Haynes, Robert M. Enick, Bret H. Howard, Dushyant Shekhawat
Summary: Hydrogen isotope separation can be achieved using a palladium (Pd) membrane due to the different solubility, diffusivity, and permeability of protium (H) and deuterium (D) in Pd. The permeability of H (k(H2)) and D (k(D2)) were studied at various temperatures and pressures using a Pd membrane separation unit. The selectivity of the Pd membrane towards H2 increases with temperature but decreases at higher temperatures due to the influence of competitive transport and isotope diffusion.
JOURNAL OF MEMBRANE SCIENCE
(2023)
Article
Chemistry, Physical
Igor Bezverkhyy, Victor Boyer, Clement Cabaud, Jean-Pierre Bellat
Summary: Quantum sieving is a promising method for the separation of hydrogen isotopes at low temperatures. This study found that the aperture size in zeolites is more important for quantum sieving than the interaction between guest cations.
ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Vladimir Vykhodets, Olga Nefedova, Tatiana Kurennykh, Sviatoslav Obukhov, Evgenia Vykhodets
Summary: This study investigates the diffusion of deuterium in potassium. It finds that mass transfer is predominantly controlled by the mechanism of overbarrier atomic jumps at temperatures 120-260 K and by the tunneling mechanism at 90-120 K. Moreover, it determines the conditions under which the quantum diffusion of hydrogen can be observed and predicts metals in which this phenomenon can be experimentally registered.
Article
Chemistry, Physical
Mostapha Dakhchoune, Luis Francisco Villalobos, Rocio Semino, Lingmei Liu, Mojtaba Rezaei, Pascal Schouwink, Claudia Esther Avalos, Paul Baade, Vanessa Wood, Yu Han, Michele Ceriotti, Kumar Varoon Agrawal
Summary: A new method for synthesizing molecular-sieving zeolitic membranes has been developed, which involves exfoliating single layers of zeolite precursor RUB-15 followed by a condensation reaction to produce thin films with high selectivity for gas separation, especially for precombustion carbon capture.
Article
Chemistry, Physical
Risako Tanii, Ryota Ogawa, Hisayoshi Matsushima, Mikito Ueda, Richard Dawson
Summary: This study investigates deuterium separation using two types of AFCs with different catalysts and finds a mass transportation limitation at Ru catalyst leading to a decrease in voltage. The slow reaction rate of D-2 gas on Ru catalyst is supported by AC impedance measurements. Experimental results show that deuterium is diluted with Pt catalyst but concentrated with Ru catalyst, possibly due to differences in adsorption energy on the catalyst surface.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Multidisciplinary Sciences
Yu Zhou, Jianlin Zhang, Lei Wang, Xili Cui, Xiaoling Liu, Sie Shing Wong, Hua An, Ning Yan, Jingyan Xie, Cong Yu, Peixin Zhang, Yonghua Du, Shibo Xi, Lirong Zheng, Xingzhong Cao, Yajing Wu, Yingxia Wang, Chongqing Wang, Haimeng Wen, Lei Chen, Huabin Xing, Jun Wang
Summary: The study successfully developed an iron-containing mordenite monolith using a template- and binder-free process, demonstrating high gas separation efficiency and stability.
Article
Materials Science, Multidisciplinary
Can Xu, Weichen Wei, Yong He
Summary: The hydrogen separation performance of molecular sieving membranes was significantly enhanced through ion exchange, showing great potential for application in hydrogen purification.
Article
Nanoscience & Nanotechnology
Junsu Ha, Minji Jung, Jaewoo Park, Hyunchul Oh, Hoi Ri Moon
Summary: This study investigates Hofmann-type metal-organic frameworks (MOFs) for hydrogen isotope separation. The results show that Co(pyz)[Pd(CN)(4)] exhibits high selectivity and capacity, making it a promising material for practical applications in isotope separation.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Environmental Sciences
Jie Liang, Wen-yu Cheng, Jing-lin Li, Xiao-chong Xue, Ke Deng, Chao-fei Liang, Lin Du, Qin Zhang, Wei Liu
Summary: By measuring the concentration of hydrogen isotopes in soil samples at different distances, the spatial distribution of tritium released from nuclear power plants can be determined. Determination of deuterium concentration in the environment may serve as a new method to trace the released tritium from reactors.
JOURNAL OF ENVIRONMENTAL RADIOACTIVITY
(2023)
Article
Engineering, Environmental
Cheng-Tong Wang, Wen-Cui Li, Shuang Xu, Ru-Shuai Liu, Guang-Ping Hao, An-Hui Lu
Summary: This study reports a wood frame structured carbon adsorbent with an integrated sieving layer, prepared from natural woods. The adsorbent exhibits excellent propylene/propane separation performance.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Applied
Renjin Xiong, Jinfan Chen, Linda Zhang, Peilong Li, Xiayan Yan, Yaqi Song, Wenhua Luo, Tao Tang, Ge Sang, Michael Hirscher
Summary: Zeolites, specifically Ag(I)-ZSM-5, have shown promising results in separating hydrogen isotopes through a strong chemical affinity quantum sieving effect. The selectivity for deuterium enrichment and separation at and above liquid nitrogen temperature was demonstrated, with a D-2/H-2 selectivity of 8.7 at 77 K. This study also predicted the hydrogen isotope selectivities under different temperatures, highlighting the potential for challenging hydrogen isotopes separation using easily scalable zeolites with controlled chemical affinity quantum sieving effect.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Chemistry, Physical
Xuanfu Zhu, Gengwu Zhang, Lukman O. Alimi, Basem M. Moosa, Abdul-Hamid Emwas, Fang Fang, Niveen M. Khashab
Summary: This study presents an energy-efficient method for the adsorptive separation of para-halotoluene (PHT) using a TI macrocycle. The selectivity is determined by the specific interactions between the macrocycle and the guest molecules. The results demonstrate the viability of using molecular sieves for sustainable chemical separation processes.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Enming Ping, Xiaoxiao Chen, Yunshan Zhou, Lijuan Zhang, Lingyun Kong, Nan Chen
Summary: In this study, CAU-10-H@gamma-AlOOH and UTSA-16@CAU-10-H@gamma-AlOOH were prepared. Cryogenic gas chromatography at 77 K using the composites achieved complete separation of o-H-2 and D-2 with CAU-10-H@gamma-AlOOH, while UTSA-16@CAU-10-H@gamma-AlOOH achieved more efficient separation of hydrogen isotopes in a shorter time. The molecular simulation results showed that CAU-10-H had both chemical affinity quantum sieving and kinetic sieving effects, while UTSA-16 only exerted the kinetic sieving effect.
INORGANIC CHEMISTRY
(2023)
Article
Engineering, Environmental
A. Gutierrez-Ortega, R. Nomen, J. Sempere, J. B. Parra, M. A. Montes-Moran, R. Gonzalez-Olmos
Summary: A new methodology for evaluating commercial adsorbents for CO2 capture using temperature swing adsorption has been developed. The study found that binderless zeolites performed better in CO2 production and desorption energy compared to their binder-based counterparts. The 13XBL binderless zeolite had the highest CO2 production and lowest desorption energy, while the 5A zeolites had the lowest CO2 production and highest desorption energy among the zeolites.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Applied
E. Acuna-Yeomans, J. J. Gutierrez-Sevillano, S. Calero, D. Dubbeldam
Summary: Metal-Organic Frameworks (MOFs) have great potential in adsorption applications due to their large pore volumes and surface areas. However, there is a lack of research on the mechanical stability of MOFs. This study investigates the elastic constants of the ZIF-8 MOF and compares different force fields and calculation methods. The results provide insights into the relationship between elastic properties and force field parametrization, and highlight the importance of energy minimization algorithms in achieving accurate results for MOFs.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Engineering, Chemical
Botagoz Zhakisheva, Juan Jose Gutierrez-Sevillano, Sofia Calero
Summary: We investigated the effect of aluminum T-position on the heat of adsorption of ammonia and water in MOR, MFI, and FAU zeolites. The results show that the T3 position has a noticeable variation for both molecules and ammonia has the strongest interaction with zeolite in this position. MFI type zeolite is also sensitive to the Al-position, especially in the case of ammonia adsorption. FAU zeolite, on the other hand, is insensitive to T-positions and has almost constant heats of adsorption for water and ammonia.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Physical
M. Munoz-Morales, A. Ramirez, Aurelien Canizares, J. Llanos, Conchi Ania
Summary: This study investigated the performance of 22 carbon materials with different origins and physicochemical characteristics as cathodes in the electrochemical production of hydrogen peroxide. Carbon nanotubes and carbon nanofibers showed the highest H2O2 production yields compared to common carbon benchmarks. Low-cost and disordered carbon cathodes with moderate electrical conductivity and density of structural defects also exhibited good catalytic activity. The structural parameters of the carbon materials were found to be more closely related to H2O2 production yield and faradaic efficiency than electrical conductivity, composition, or porous features. An AD/AG threshold value of 1.5 can be used to discriminate the electrocatalytic activity of carbon cathodes for H2O2 production.
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, Physical
Shrinjay Sharma, Marcello S. S. Rigutto, Richard Baur, Umang Agarwal, Erik Zuidema, Salvador R. G. Balestra, Sofia Calero, David Dubbeldam, Thijs J. H. Vlugt
Summary: Ideal Adsorbed Solution Theory (IAST) is a common method for modeling mixture adsorption isotherms, while the segregated version (SIAST) provides improved adsorbed loadings. We have adopted the concept of SIAST and developed the Segregated Explicit Isotherm (SEI) model which considers both size-effects of co-adsorbed molecules and surface heterogeneities. Compared to IAST and SIAST, SEI does not require an iterative scheme, resulting in faster simulations with excellent agreement with experimental data.
Article
Chemistry, Physical
Shrinjay Sharma, Salvador R. G. Balestra, Richard Baur, Umang Agarwal, Erik Zuidema, Marcello S. Rigutto, Sofia Calero, Thijs J. H. Vlugt, David Dubbeldam
Summary: The RUPTURA code is introduced as a free and open-source software package for gas adsorption simulation, mixture prediction, and isotherm model fitting. It can be combined with the RASPA software to compute breakthrough curves directly from adsorption simulations. The code supports a variety of isotherm models and provides an easy way to obtain the model parameters through the fitting module.
MOLECULAR SIMULATION
(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
Chemistry, Multidisciplinary
Rafael M. Madero-Castro, Azahara Luna-Triguero, Andrzej Slawek, Jose Manuel Vicent-Luna, Sofia Calero
Summary: This paper investigates the adsorption of polar working fluids in hydrophobic and hydrophilic zeolites for thermal energy storage applications. Experimental and simulated adsorption isotherms of water and methanol in high-silica HS-FAU, NaY, and NaX zeolites were obtained. The results were used to develop a parameter model for the interaction between methanol and the zeolite and cations. The performance of the adsorbate working fluids for heat storage was evaluated using a mathematical model based on Dubinin-Polanyi adsorption potential theory. The importance of controlling the hydrophilic/hydrophobic nature of zeolites by changing the Al content was highlighted.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(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, 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)
Review
Chemistry, Multidisciplinary
Bipasa Samanta, Angel Morales-Garcia, Francesc Illas, Nicolae Goga, Juan Antonio Anta, Sofia Calero, Anja Bieberle-Hutter, Florian Libisch, Ana B. Munoz-Garcia, Michele Pavone, Maytal Caspary Toroker
Summary: Understanding the water splitting mechanism in photocatalysis is crucial for producing clean fuel in the future. Different theoretical methods at various scales have strengths and drawbacks, and a combination of methods is needed to model complex nano-photocatalysts accurately.
CHEMICAL SOCIETY REVIEWS
(2022)