19 results on '"Snurr, Randall Q."'
Search Results
2. Progress toward the computational discovery of new metal–organic framework adsorbents for energy applications.
- Author
-
Moghadam, Peyman Z., Chung, Yongchul G., and Snurr, Randall Q.
- Published
- 2024
- Full Text
- View/download PDF
3. Regulating adsorption performance of zeolites by pre-activation in electric fields.
- Author
-
Chen, Kaifei, Yu, Zhi, Mousavi, Seyed Hesam, Singh, Ranjeet, Gu, Qinfen, Snurr, Randall Q., Webley, Paul A., and Li, Gang Kevin
- Subjects
GAS absorption & adsorption ,ADSORPTION (Chemistry) ,ADSORPTION capacity ,ZEOLITES ,MOLECULAR sieves - Abstract
While multiple external stimuli (e.g., temperature, light, pressure) have been reported to regulate gas adsorption, limited studies have been conducted on controlling molecular admission in nanopores through the application of electric fields (E-field). Here we show gas adsorption capacity and selectivity in zeolite molecular sieves can be regulated by an external E-field. Through E-field pre-activation during degassing, several zeolites exhibited enhanced CO
2 adsorption and decreased CH4 and N2 adsorptions, improving the CO2 /CH4 and CO2 /N2 separation selectivity by at least 25%. The enhanced separation performance of the zeolites pre-activated by E-field was maintained in multiple adsorption/desorption cycles. Powder X-ray diffraction analysis and ab initio computational studies revealed that the cation relocation and framework expansion induced by the E-field accounted for the changes in gas adsorption capacities. These findings demonstrate a regulation approach to sharpen the molecular sieving capability by E-fields and open new avenues for carbon capture and molecular separations. The gas adsorption capacity and selectivity in zeolite molecular sieves can be regulated by an external electric field through the electric field-induced cation relocation and framework expansion. [ABSTRACT FROM AUTHOR]- Published
- 2023
- Full Text
- View/download PDF
4. Computational investigation of hysteresis and phase equilibria of n-alkanes in a metal-organic framework with both micropores and mesopores.
- Author
-
Li, Zhao, Turner, Jake, and Snurr, Randall Q.
- Subjects
PHASE equilibrium ,METAL-organic frameworks ,MESOPORES ,ADSORBATES ,POROUS materials ,ADSORPTION isotherms ,HYSTERESIS ,MICROPORES - Abstract
Adsorption hysteresis is a phenomenon related to phase transitions that can impact applications such as gas storage and separations in porous materials. Computational approaches can greatly facilitate the understanding of phase transitions and phase equilibria in porous materials. In this work, adsorption isotherms for methane, ethane, propane, and n-hexane were calculated from atomistic grand canonical Monte Carlo (GCMC) simulations in a metal-organic framework having both micropores and mesopores to better understand hysteresis and phase equilibria between connected pores of different size and the external bulk fluid. At low temperatures, the calculated isotherms exhibit sharp steps accompanied by hysteresis. As a complementary simulation method, canonical (NVT) ensemble simulations with Widom test particle insertions are demonstrated to provide additional information about these systems. The NVT+Widom simulations provide the full van der Waals loop associated with the sharp steps and hysteresis, including the locations of the spinodal points and points within the metastable and unstable regions that are inaccessible to GCMC simulations. The simulations provide molecular-level insight into pore filling and equilibria between high- and low-density states within individual pores. The effect of framework flexibility on adsorption hysteresis is also investigated for methane in IRMOF-1. Developing computational tools to study the phase behaviour of adsorbate molecules in complex pore architectures can greatly facilitate our understanding of phase transitions and phase equilibria in porous materials. Here, molecular simulations are used to study the hysteresis and phase equilibria of n-alkane adsorbate molecules in a metal–organic framework with both micropores and mesopores, and simulations in the canonical ensemble with Widom insertions are shown to be a powerful complementary approach to grand canonical Monte Carlo simulations. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
5. Applying design principles to improve hydrogen storage capacity in nanoporous materials.
- Author
-
Bobbitt, N. Scott, Li, Eric, and Snurr, Randall Q.
- Published
- 2022
- Full Text
- View/download PDF
6. Connecting theory and simulation with experiment for the study of diffusion in nanoporous solids
- Author
-
Bukowski, Brandon C., Keil, Frerich J., Ravikovitch, Peter I., Sastre, Germán, Snurr, Randall Q., Coppens, Marc-Olivier, Ministerio de Ciencia e Innovación (España), and Ministerio de Economía y Competitividad (España)
- Abstract
Nanoporous solids are ubiquitous in chemical, energy, and environmental processes, where controlled transport of molecules through the pores plays a crucial role. They are used as sorbents, chromatographic or membrane materials for separations, and as catalysts and catalyst supports. Defined as materials where confinement effects lead to substantial deviations from bulk diffusion, nanoporous materials include crystalline microporous zeotypes and metal–organic frameworks (MOFs), and a number of semi-crystalline and amorphous mesoporous solids, as well as hierarchically structured materials, containing both nanopores and wider meso- or macropores to facilitate transport over macroscopic distances. The ranges of pore sizes, shapes, and topologies spanned by these materials represent a considerable challenge for predicting molecular diffusivities, but fundamental understanding also provides an opportunity to guide the design of new nanoporous materials to increase the performance of transport limited processes. Remarkable progress in synthesis increasingly allows these designs to be put into practice. Molecular simulation techniques have been used in conjunction with experimental measurements to examine in detail the fundamental diffusion processes within nanoporous solids, to provide insight into the free energy landscape navigated by adsorbates, and to better understand nano-confinement effects. Pore network models, discrete particle models and synthesis-mimicking atomistic models allow to tackle diffusion in mesoporous and hierarchically structured porous materials, where multiscale approaches benefit from ever cheaper parallel computing and higher resolution imaging. Here, we discuss synergistic combinations of simulation and experiment to showcase theoretical progress and computational techniques that have been successful in predicting guest diffusion and providing insights. We also outline where new fundamental developments and experimental techniques are needed to enable more accurate predictions for complex systems. BCB and RQS acknowledge support from the Defense Threat Reduction Agency (HDTRA1-19-1-0007). MOC gratefully acknowledges support from the EPSRC via “Frontier Engineering” and “Frontier Engineering: Progression” Awards (EP/K038656/1, EP/S03305X/1). GS thanks MICINN of Spain for funding through projects RTI2018-101784-B-I00, RTI2018-101033-B-I00, SEV-2016-0683.
- Published
- 2021
7. High-throughput predictions of metal–organic framework electronic properties: theoretical challenges, graph neural networks, and data exploration.
- Author
-
Rosen, Andrew S., Fung, Victor, Huck, Patrick, O'Donnell, Cody T., Horton, Matthew K., Truhlar, Donald G., Persson, Kristin A., Notestein, Justin M., and Snurr, Randall Q.
- Subjects
BAND gaps ,METAL-organic frameworks ,ATOMIC charges ,ELECTRON density ,ELECTRONIC structure - Abstract
With the goal of accelerating the design and discovery of metal–organic frameworks (MOFs) for electronic, optoelectronic, and energy storage applications, we present a dataset of predicted electronic structure properties for thousands of MOFs carried out using multiple density functional approximations. Compared to more accurate hybrid functionals, we find that the widely used PBE generalized gradient approximation (GGA) functional severely underpredicts MOF band gaps in a largely systematic manner for semi-conductors and insulators without magnetic character. However, an even larger and less predictable disparity in the band gap prediction is present for MOFs with open-shell 3d transition metal cations. With regards to partial atomic charges, we find that different density functional approximations predict similar charges overall, although hybrid functionals tend to shift electron density away from the metal centers and onto the ligand environments compared to the GGA point of reference. Much more significant differences in partial atomic charges are observed when comparing different charge partitioning schemes. We conclude by using the dataset of computed MOF properties to train machine-learning models that can rapidly predict MOF band gaps for all four density functional approximations considered in this work, paving the way for future high-throughput screening studies. To encourage exploration and reuse of the theoretical calculations presented in this work, the curated data is made publicly available via an interactive and user-friendly web application on the Materials Project. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
8. Inverse design of nanoporous crystalline reticular materials with deep generative models.
- Author
-
Yao, Zhenpeng, Sánchez-Lengeling, Benjamín, Bobbitt, N. Scott, Bucior, Benjamin J., Kumar, Sai Govind Hari, Collins, Sean P., Burns, Thomas, Woo, Tom K., Farha, Omar K., Snurr, Randall Q., and Aspuru-Guzik, Alán
- Published
- 2021
- Full Text
- View/download PDF
9. Impact of H2O and CO2 on methane storage in metal–organic frameworks.
- Author
-
Gonçalves, Daniel V., Snurr, Randall Q., and Lucena, Sebastião M. P.
- Abstract
We investigated eight representative metal–organic frameworks for methane storage using molecular simulation. Validated force fields were used to calculate the amount adsorbed for pure methane and its mixtures with CO2 and H2O at 5.8 and 65 bar at 298 K within the composition limits specified for natural gas. Within the analyzed concentrations, the MOFs without open metal sites were minimally influenced by the presence of CO2 and H2O. However, for the MOFs with open metal sites, the presence of these species proved to be harmful. We found that concentrations as low as 25 ppm of water can reduce the delivered volume of methane by more than 20%. A detailed analysis of the adsorption mechanisms leading to this poisoning is presented. These results highlight the possible limitations of MOFs with open metal sites for use in natural gas storage. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
10. A molecular flip-flop for separating heavy water.
- Author
-
Heine, Thomas and Snurr, Randall Q.
- Abstract
Molecules of heavy water contain the deuterium isotope of hydrogen and have been impossible to separate from ordinary water. Nanoporous materials with flexible apertures in their structures point the way to a solution.A material that preferentially adsorbs one isotopic analogue of water. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
11. Computer-aided discovery of a metal–organic framework with superior oxygen uptake.
- Author
-
Moghadam, Peyman Z., Fantham, Marcus, Kaminski, Clemens F., Fairen-Jimenez, David, Islamoglu, Timur, Goswami, Subhadip, Farha, Omar K., Exley, Jason, and Snurr, Randall Q.
- Subjects
METAL activation ,ACTIVATION (Chemistry) ,OXYGEN ,CHALCOGENS ,NONMETALS - Abstract
Current advances in materials science have resulted in the rapid emergence of thousands of functional adsorbent materials in recent years. This clearly creates multiple opportunities for their potential application, but it also creates the following challenge: how does one identify the most promising structures, among the thousands of possibilities, for a particular application? Here, we present a case of computer-aided material discovery, in which we complete the full cycle from computational screening of metal–organic framework materials for oxygen storage, to identification, synthesis and measurement of oxygen adsorption in the top-ranked structure. We introduce an interactive visualization concept to analyze over 1000 unique structure–property plots in five dimensions and delimit the relationships between structural properties and oxygen adsorption performance at different pressures for 2932 alreadysynthesized structures. We also report a world-record holding material for oxygen storage, UMCM-152, which delivers 22.5% more oxygen than the best known material to date, to the best of our knowledge. [ABSTRACT FROM AUTHOR]
- Published
- 2018
- Full Text
- View/download PDF
12. Large-Scale Generation and Screening of Hypothetical Metal-Organic Frameworks for Applications in Gas Storage and Separations.
- Author
-
Wilmer, Christopher E. and Snurr, Randall Q.
- Published
- 2014
- Full Text
- View/download PDF
13. Destruction of chemical warfare agents using metal-organic frameworks.
- Author
-
Mondloch, Joseph E., Katz, Michael J., Isley III, William C., Ghosh, Pritha, Liao, Peilin, Bury, Wojciech, Wagner, George W., Hall, Morgan G., DeCoste, Jared B., Peterson, Gregory W., Snurr, Randall Q., Cramer, Christopher J., Hupp, Joseph T., and Farha, Omar K.
- Subjects
CHEMICAL warfare agents ,METAL-organic frameworks ,POROSITY ,LEWIS acids ,ZIRCONIUM ,CHEMICAL stability - Abstract
Chemical warfare agents containing phosphonate ester bonds are among the most toxic chemicals known to mankind. Recent global military events, such as the conflict and disarmament in Syria, have brought into focus the need to find effective strategies for the rapid destruction of these banned chemicals. Solutions are needed for immediate personal protection (for example, the filtration and catalytic destruction of airborne versions of agents), bulk destruction of chemical weapon stockpiles, protection (via coating) of clothing, equipment and buildings, and containment of agent spills. Solid heterogeneous materials such as modified activated carbon or metal oxides exhibit many desirable characteristics for the destruction of chemical warfare agents. However, low sorptive capacities, low effective active site loadings, deactivation of the active site, slow degradation kinetics, and/or a lack of tailorability offer significant room for improvement in these materials. Here, we report a carefully chosen metal-organic framework (MOF) material featuring high porosity and exceptional chemical stability that is extraordinarily effective for the degradation of nerve agents and their simulants. Experimental and computational evidence points to Lewis-acidic Zr
IV ions as the active sites and to their superb accessibility as a defining element of their efficacy. [ABSTRACT FROM AUTHOR]- Published
- 2015
- Full Text
- View/download PDF
14. Large-scale screening of hypothetical metal-organic frameworks.
- Author
-
Wilmer, Christopher E., Leaf, Michael, Lee, Chang Yeon, Farha, Omar K., Hauser, Brad G., Hupp, Joseph T., and Snurr, Randall Q.
- Subjects
METHANE ,ORGANOMETALLIC compounds ,CHEMICAL libraries ,MEDICAL screening ,METHANE hydrates ,DIAZOMETHANE - Abstract
Metal-organic frameworks (MOFs) are porous materials constructed from modular molecular building blocks, typically metal clusters and organic linkers. These can, in principle, be assembled to form an almost unlimited number of MOFs, yet materials reported to date represent only a tiny fraction of the possible combinations. Here, we demonstrate a computational approach to generate all conceivable MOFs from a given chemical library of building blocks (based on the structures of known MOFs) and rapidly screen them to find the best candidates for a specific application. From a library of 102 building blocks we generated 137,953 hypothetical MOFs and for each one calculated the pore-size distribution, surface area and methane-storage capacity. We identified over 300 MOFs with a predicted methane-storage capacity better than that of any known material, and this approach also revealed structure-property relationships. Methyl-functionalized MOFs were frequently top performers, so we selected one such promising MOF and experimentally confirmed its predicted capacity. [ABSTRACT FROM AUTHOR]
- Published
- 2012
- Full Text
- View/download PDF
15. De novo synthesis of a metal-organic framework material featuring ultrahigh surface area and gas storage capacities.
- Author
-
Farha, Omar K., Özgür Yazaydın, A., Eryazici, Ibrahim, Malliakas, Christos D., Hauser, Brad G., Kanatzidis, Mercouri G., Nguyen, SonBinh T., Snurr, Randall Q., and Hupp, Joseph T.
- Subjects
METAL ions ,STRUCTURAL frames ,POROUS materials ,BLOCKS (Building materials) ,SURFACE area ,ABSORPTION ,HYDROGEN ,ORGANIC conductors ,CARBON dioxide - Abstract
Metal-organic frameworks-a class of porous hybrid materials built from metal ions and organic bridges-have recently shown great promise for a wide variety of applications. The large choice of building blocks means that the structures and pore characteristics of the metal-organic frameworks can be tuned relatively easily. However, despite much research, it remains challenging to prepare frameworks specifically tailored for particular applications. Here, we have used computational modelling to design and predictively characterize a metal-organic framework (NU-100) with a particularly high surface area. Subsequent experimental synthesis yielded a material, matching the calculated structure, with a high BET surface area (6,143 m
2 g−1 ). Furthermore, sorption measurements revealed that the material had high storage capacities for hydrogen (164 mg g−1 ) and carbon dioxide (2,315 mg g−1 )-gases of high importance in the contexts of clean energy and climate alteration, respectively-in excellent agreement with predictions from modelling. [ABSTRACT FROM AUTHOR]- Published
- 2010
- Full Text
- View/download PDF
16. Investigation of particle damping mechanism via particle dynamics simulations.
- Author
-
Xian-Ming Bai, Keer, Leon M., Wang, Q. Jane, and Snurr, Randall Q.
- Subjects
DAMPING (Mechanics) ,MOLECULAR dynamics ,PARTICLES (Nuclear physics) ,TRIBOLOGY ,ENERGY storage - Abstract
Damping systems using granular particles as the damping medium are promising for application in extreme temperature conditions. In particle-based damping systems, mechanical energy is dissipated through inelastic collisions and friction between particles. In this work, we use particle dynamics simulations to investigate and compare the damping mechanisms of a piston-type thrust damper and a box-type oscillation damper. The mechanisms of energy transfer and energy dissipation are investigated. The roles of friction and inelastic collisions, as well as the wall effects in energy dissipation, are examined. The simulation results provide better understanding of the particle damping mechanisms, which may help in the design of next generation particle damping devices. [ABSTRACT FROM AUTHOR]
- Published
- 2009
- Full Text
- View/download PDF
17. Connecting theory and simulation with experiment for the study of diffusion in nanoporous solids
- Abstract
Nanoporous solids are ubiquitous in chemical, energy, and environmental processes, where controlled transport of molecules through the pores plays a crucial role. They are used as sorbents, chromatographic or membrane materials for separations, and as catalysts and catalyst supports. Defined as materials where confinement effects lead to substantial deviations from bulk diffusion, nanoporous materials include crystalline microporous zeotypes and metal–organic frameworks (MOFs), and a number of semi-crystalline and amorphous mesoporous solids, as well as hierarchically structured materials, containing both nanopores and wider meso- or macropores to facilitate transport over macroscopic distances. The ranges of pore sizes, shapes, and topologies spanned by these materials represent a considerable challenge for predicting molecular diffusivities, but fundamental understanding also provides an opportunity to guide the design of new nanoporous materials to increase the performance of transport limited processes. Remarkable progress in synthesis increasingly allows these designs to be put into practice. Molecular simulation techniques have been used in conjunction with experimental measurements to examine in detail the fundamental diffusion processes within nanoporous solids, to provide insight into the free energy landscape navigated by adsorbates, and to better understand nano-confinement effects. Pore network models, discrete particle models and synthesis-mimicking atomistic models allow to tackle diffusion in mesoporous and hierarchically structured porous materials, where multiscale approaches benefit from ever cheaper parallel computing and higher resolution imaging. Here, we discuss synergistic combinations of simulation and experiment to showcase theoretical progress and computational techniques that have been successful in predicting guest diffusion and providing insights. We also outline where new fundamental developments and experimental techniques are needed t
- Published
- 2021
18. Quantum Chemical Determination of Stable Intermediates on CO Adsorption Onto Metal(Salen) Complexes.
- Author
-
Curet-Arana, Maria, Meza, Paul, Irizarry, Radames, and Soler, Rafael
- Subjects
COBALT ,ADSORPTION (Chemistry) ,QUANTUM chemistry ,CHEMICAL stability ,METAL complexes ,COUPLING reactions (Chemistry) ,POLYCARBONATES ,CHEMICAL reactions - Abstract
Coupling reactions of CO and epoxides to produce either cyclic carbonates or polycarbonates are environmentally friendly reactions that allow the use of an inexpensive and renewable feedstock while achieving carbon efficiency. In this study, density functional theory calculations were used to understand the role the metal(salen) catalyst on CO adsorption. We have performed a systematic analysis of the plausible interactions of CO with metal(salen) catalysts and ethylene oxide/metal(salen) complexes. Adsorption reactions were analyzed on six metal(salen) complexes: Co, Cr, Mn, Fe, Zn, and Al, using the unrestricted OPBE functional. Geometry optimizations were carried out beginning with a variety of different conformations and frequency calculations were used to verify that structures lie in an energy minimum. Our results demonstrate that CO does not bind to the metal atom of the bare metal(salen). The adsorption of CO onto metal(salen) complexes is an endothermic reaction and the lowest energy adsorbed complex involves the interaction of CO with the adsorbed opened-epoxide. [ABSTRACT FROM AUTHOR]
- Published
- 2012
- Full Text
- View/download PDF
19. Insight into Fluorocarbon Adsorption in Metal-Organic Frameworks via Experiments and Molecular Simulations.
- Author
-
Barpaga, Dushyant, Nguyen, Van T., Medasani, Bharat K., Chatterjee, Sayandev, McGrail, B. Peter, Motkuri, Radha Kishan, and Dang, Liem X.
- Abstract
The improvement in adsorption/desorption of hydrofluorocarbons has implications for many heat transformation applications such as cooling, refrigeration, heat pumps, power generation, etc. The lack of chlorine in hydrofluorocarbons minimizes the lasting environmental damage to the ozone, with R134a (1,1,1,2-tetrafluoroethane) being used as the primary industrial alternative to commonly used Freon-12. The efficacy of novel adsorbents used in conjunction with R134a requires a deeper understanding of the host-guest chemical interaction. Metal-organic frameworks (MOFs) represent a newer class of adsorbent materials with significant industrial potential given their high surface area, porosity, stability, and tunability. In this work, we studied two benchmark MOFs, a microporous Ni-MOF-74 and mesoporous Cr-MIL-101. We employed a combined experimental and simulation approach to study the adsorption of R134a to better understand host-guest interactions using equilibrium isotherms, enthalpy of adsorption, Henry's coefficients, and radial distribution functions. The overall uptake was shown to be exceptionally high for Cr-MIL-101, >140 wt% near saturation while >50 wt% at very low partial pressures. For both MOFs, simulation data suggest that metal sites provide preferable adsorption sites for fluorocarbon based on favorable C-F ··· M
+ interactions between negatively charged fluorine atoms of R134a and positively charged metal atoms of the MOF framework. [ABSTRACT FROM AUTHOR]- Published
- 2019
- Full Text
- View/download PDF
Catalog
Discovery Service for Jio Institute Digital Library
For full access to our library's resources, please sign in.