Combined Nuclear Magnetic Resonance and Molecular Dynamics Study of Methane Adsorption in M<sub>2</sub>(dobdc) Metal–Organic Frameworks

Witherspoon, Velencia J.; Mercado, Rocío; Braun, Efrem; Mace, Amber; Bachman, Jonathan E.; Blümich, Bernhard; Smit, Berend; Reimer, Jeffrey A.

doi:10.1021/acs.jpcc.9b01733

Cited by 23 publications

(16 citation statements)

References 54 publications

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“…It was found that the self‐diffusion coefficient of methane in M 2 (dobdc) was inversely related to the binding energy at the unsaturated metal sites. [ 80 ]…”

Section: Ssnmr Characterization Of Mofsmentioning

confidence: 99%

Recent Advances of Solid‐State NMR Spectroscopy for Microporous Materials

Lafon

Wang

et al. 2020

Advanced Materials

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< 2 nm), such as zeolites, metal-organic frameworks (MOFs), covalent organic frameworks (COFs), and porous aromatic frameworks (PAFs), combine high specific surface areas, large pore volumes and shape-selectivity effects, which makes them key materials for a wide range of applications, including catalysis, gas separation/purification, ion exchange, gas storage, and sensing. The diverse framework compositions and functionalities of microporous materials represent a huge challenge for their structural characterization as well as evaluation of their performances. Analytic tools such as X-ray diffraction (XRD), electron microscopy and adsorption-desorption isotherms are now routinely employed for characterization of microporous materials in order to establish the structure-property relationships, and hence, to facilitate the rational design of advanced materials with improved property. However, the structure determination of porous materials using single crystal XRD requires high crystallinity and long-range ordering of the framework. Solid-state NMR (SSNMR) has emerged as a powerful spectroscopic technique with atomic-level resolution, complementary to XRD, in the investigation of structures in Microporous materials have attracted a rapid growth of research interest in materials science and the multidisciplinary area because of their wide applications in catalysis, separation, ion exchange, gas storage, drug release, and sensing. A fundamental understanding of their diverse structures and properties is crucial for rational design of high-performance materials and technological applications in industry. Solid-state NMR (SSNMR), capable of providing atomic-level information on both structure and dynamics, is a powerful tool in the scientific exploration of solid materials. Here, advanced SSNMR instruments and methods for characterization of microporous materials are briefly described. The recent progress of the application of SSNMR for the investigation of microporous materials including zeolites, metal-organic frameworks, covalent organic frameworks, porous aromatic frameworks, and layered materials is discussed with representative work. The versatile SSNMR techniques provide detailed information on the local structure, dynamics, and chemical processes in the confined space of porous materials. The challenges and prospects in SSNMR study of microporous and related materials are discussed.

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“…It was found that the self‐diffusion coefficient of methane in M 2 (dobdc) was inversely related to the binding energy at the unsaturated metal sites. [ 80 ]…”

Section: Ssnmr Characterization Of Mofsmentioning

confidence: 99%

Recent Advances of Solid‐State NMR Spectroscopy for Microporous Materials

Lafon

Wang

et al. 2020

Advanced Materials

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“…We studied the diffusion properties for selected MOFs and zeolites at low loading, and, furthermore, we also applied a new approach to investigate the diffusion in the limit of zero For this case study, we used the same structures and the same LAMMPS files, adopting the same simulation conditions as Witherspoon et al, 14 and repeated the simulations of the diffusion of CH 4 molecules at low loading inside three M 2 (dobdc) structures (M: Mg, Ni, and Zn) at 313 K.…”

Section: Resultsmentioning

confidence: 99%

“…To approach the zero loading limit, one typically tries to reduce the number of molecules and/or increase the size of the simulation cell. This work was triggered by some recent work of Witherspoon et al, 14 who have used a combination of NMR and MD simulations to study the CH 4 diffusion and their binding at the coordinatively unsaturated metal sites in M 2 (dobdc) (M = Mg, Ni, and Zn) frameworks at low and high guests' loading. At low loading, Witherspoon et al observed in the molecular dynamics simulation that the self-diffusion coefficient slowly increases until it reaches a maximum.…”

Section: Introductionmentioning

confidence: 99%

On the effects of the degrees of freedom on calculating diffusion properties in nanoporous materials

Cabriolu

Smit

2022

Preprint

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If one carries out a molecular simulation of N particles using periodic boundary conditions, linear momentum is conserved and hence the number of degrees of freedom is set to 3N-3. In most programs, this number of degrees of freedom is the default setting. However, if one carries out a molecular simulation in an external field, one needs to ensure that degrees of freedom are changed from this default setting to 3N, as in an external field the velocity of the center of mass can change. Using the correct degrees of freedom is important in calculating the temperature and in some algorithms to simulate at constant temperature. For sufficiently large systems, the difference between 3N and 3N-3 is negligible in the way. However, there are systems in which the comparison with experimental data requires molecular dynamics simulations of a small number of particles. In this work, we illustrate the effect of an incorrect setting of degrees of freedom in molecular dynamic simulations studying the diffusion properties of guest molecules in nanoporous materials. We show that previously published results have reported a surprising diffusion dependence on the loading, which could be traced back to an incorrect setting of the degrees of freedom. As the correct settings are convoluted and counter-intuitive in some of the most commonly used molecular dynamics programs, we carried out a systematic study on the consequences of the various commonly used (incorrect) settings. Our conclusion, is that for systems smaller than 50 particles the results are most likely unreliable as these are either performed at an incorrect temperature or the temperature is incorrectly used in some of the results. Furthermore, a novel and efficient method to calculate diffusion coefficients of guest molecules into nanoporous materials at zero loading conditions is introduced.

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“…There are a lot of software package for MD simulation, including Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS) [35], Chemistry at Harvard Macromolecular Mechanics (CHARMM) [36], Groningen Machine for Chemical Simulations (GROMACS) [37], Nanoscale Molecular Dynamics (NAMD) [38], Assisted Model Building with Energy Refinement (AMBER) [39], Desmond [40], Tinker [40], DL_POLY [41] and others which can be used subjected to the simulation result needed. LAMMPS software by Sandia National Laboratories was applied to simulate the nanoreinforced solder paste environment.…”

Section: Methodology 21 MD Simulation Via Lammpsmentioning

confidence: 99%

Investigation of Nano-Reinforced Lead-Free Solder During Reflow Soldering-A Molecular Dynamic Approach

Sahrudin

Abdullah

Aziz

et al. 2020

CFDL

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The reinforcement of nanoparticles into the lead-free solder is proved to give good increment in the result of the importance solder properties which includes wetting properties and mechanical properties. This study proposed the new simulation method for the nano-reinforced solder to investigate the complexity and atomic behaviour briefly. The objective of this study is to clearly show the movement of the reinforced nanoparticles in the solder during the reflow soldering process via molecular dynamics (MD) simulation. In this work, Nickel (Ni) nanoparticles will be added into the pure Tin (Sn) lead-free solder. The MD simulation of Ni-reinforced solder at the temperature of 250 OC (reflow phase) was conducted via Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS) software. This simulation model able to track the nanoparticles movement in the solder during the reflow soldering process. The experimental procedure of 0.01 wt.% Ni nanoparticle reinforcement in Sn100C was also carried out to validate the simulation result. The synchrotron micro-XRF mapping showed the Ni element was agglomerated and thus validated the simulation result. The measured area of agglomerated Ni A in the simulation and experimental results are 1.1708 Å2 and 0.9996 Å2, respectively. Meanwhile, the result obtained for area B is 0.7696 Å2 and 0.6796 Å2, respectively. Therefore, the percentage error of simulation and experimental results for both areas of A and B is 10.82% and 13.24%, respectively.

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Combined Nuclear Magnetic Resonance and Molecular Dynamics Study of Methane Adsorption in M₂(dobdc) Metal–Organic Frameworks

Cited by 23 publications

References 54 publications

Recent Advances of Solid‐State NMR Spectroscopy for Microporous Materials

Recent Advances of Solid‐State NMR Spectroscopy for Microporous Materials

On the effects of the degrees of freedom on calculating diffusion properties in nanoporous materials

Investigation of Nano-Reinforced Lead-Free Solder During Reflow Soldering-A Molecular Dynamic Approach

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Combined Nuclear Magnetic Resonance and Molecular Dynamics Study of Methane Adsorption in M2(dobdc) Metal–Organic Frameworks

Cited by 23 publications

References 54 publications

Recent Advances of Solid‐State NMR Spectroscopy for Microporous Materials

Recent Advances of Solid‐State NMR Spectroscopy for Microporous Materials

On the effects of the degrees of freedom on calculating diffusion properties in nanoporous materials

Investigation of Nano-Reinforced Lead-Free Solder During Reflow Soldering-A Molecular Dynamic Approach

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Product

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Combined Nuclear Magnetic Resonance and Molecular Dynamics Study of Methane Adsorption in M₂(dobdc) Metal–Organic Frameworks