Computational Study on the Influences of Framework Charges on CO<sub>2</sub> Uptake in Metal−Organic Frameworks

Zheng, Chengcheng; Liu, Dahuan; Yang, Qingyuan; Zhong, Chongli; Mi, Jianguo

doi:10.1021/ie901000x

Cited by 76 publications

(59 citation statements)

References 32 publications

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“…[14][15][16] At present, many studies have been carried out on the adsorption and diffusion of pure gases in ZIFs. [8][9][10][11][12][13][14][15][16][17][18][19][20] Experimentally, for example, Yaghi and co-workers measured the adsorption isotherms of CO 2 , CO, CH 4 , N 2 , and O 2 in several ZIFs. [14][15][16] Wu et al 13 studied the H 2 adsorption sites and binding energies in ZIF-8 using a combined experimental and computational method.…”

Section: Introductionmentioning

confidence: 99%

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Molecular Simulation Studies of Separation of CO₂/N₂, CO₂/CH₄, and CH₄/N₂ by ZIFs

2010

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In this work, molecular simulations were performed to evaluate the separation performance of two typical zeolitic imidazolate frameworks (ZIFs), ZIF-68 and ZIF-69, for CO 2 /N 2 , CO 2 /CH 4 , and CH 4 /N 2 mixtures. To do this, we first identified a suitable force field for describing CO 2 , N 2 , and CH 4 adsorption in ZIFs. On the basis of the validated force field, adsorption selectivities of the three mixtures in these ZIFs were simulated then. The results show that ZIF-69 is more beneficial for separating CO 2 from CO 2 -related mixtures than ZIF-68, mainly due to the presence of chlorine atoms in cbIM linkers in the former for the pressures we have considered. The overall separation performances of these two ZIFs for separating the chosen mixtures are comparable to typical MOFs and zeolites. In addition, this work demonstrates that the electrostatic interactions produced by the frameworks are very important for achieving high adsorption separation selectivities in ZIFs, and ideal adsorbed solution theory (IAST) may be applicable to ZIFs. Furthermore, the effect of water on the separation performance of the two ZIFs was also investigated.

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Section: Introductionmentioning

confidence: 99%

“…17 They also studied the influences of framework charges on CO 2 uptake in some ZIFs. 18 Johnson and co-workers computed the adsorption and diffusion of CO 2 , N 2 , CH 4 , and H 2 in ZIF-68 and ZIF-70 from atomistic simulations. 19 Zhou et al 20 employed grand canonical Monte Carlo (GCMC) simulations to study hydrogen adsorption in ZIF-8.…”

Section: Introductionmentioning

confidence: 99%

Molecular Simulation Studies of Separation of CO₂/N₂, CO₂/CH₄, and CH₄/N₂ by ZIFs

2010

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“…Zheng et al 14 investigated the influence of framework charges on the CO 2 uptake in MOFs and demonstrated that the framework charge contribution in MOFs cannot be ignored in computational screening of MOF materials for CO 2 capture. Currently, several strategies for calculating atomic charges of the MOFs are available.…”

Section: Introductionmentioning

confidence: 99%

Accurate Ab Initio-Based Force Field for Predictive CO₂ Uptake Simulations in MOFs and ZIFs: Development and Applications for MTV-MOFs

et al. 2012

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For a reliable prediction of CO 2 loading in metal−organic (MOFs) and zeolitic-imidazolate frameworks (ZIFs) by molecular simulation, accurate description of the van der Waals (vdW) and Coulomb interactions is undoubtedly the most critical component. However, there have been some strong recent indications that the use of generic force fields (FFs) widely used in most current CO 2 / MOF simulations that were not particularly parametrized for CO 2 /MOF and ZIF systems could lead to serious discrepancies compared to experimental results. Here, we develop accurate vdW FFs for CO 2 uptake simulations in MOFs and ZIFs using high-level ab initio calculations, and validate the method by comparing the simulated and experimental CO 2 uptakes for various known MOFs and ZIFs. The agreements between simulations and experiments are shown to be excellent for several known MOFs and ZIFs, although the FF parameters are not specifically fitted to those particular systems, showing the potential transferability of the FF. Atomic charges of the adsorbents are computed via the rapid charge equilibration method. Using these highly accurate FFs, we reveal the origin of the enhanced CO 2 uptake in recently reported MOFs having multivariate functional groups (MTV-MOFs). We find that the capacity enhancement in MTV-MOFs arises from an increase in both vdW (due to tighter geometry) and electrostatic (due to increased dipole moment) interactions between CO 2 and MTV-MOF. We further predict that MOF-5-NO 2 can have an even higher CO 2 uptake than these MTV-MOFs due to a larger local dipole moment of the NO 2 -functionalized linker than those found in the reported MTV-MOFs. As a further designing of the high capacity material, we then introduced both electron-donating and -withdrawing functional groups simultaneously in the same organic linker to increase the local dipole moment of the linker significantly. The resulting CO 2 uptake indeed increases substantially due to the favorable electrostatic interactions that can be tested experimentally.

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“…Some researchers also studied the absorption capacity of methylimidazole [15][16][17] and the adsorption capacity of methylimidazole with porous materials [18][19][20] for the carbon dioxide molecule. The potential of methylimidazole for capturing carbon dioxide molecules was reported.…”

Section: Introductionmentioning

confidence: 99%

Separation of Methane and Carbon Dioxide Gas Mixtures Using Activated Carbon Modified with 2‐Methylimidazole

et al. 2018

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Activated carbon was modified by loading 2-methylimidazole (mIm), ethanol, and glycol onto its surface and adopted to capture CO 2 using the absorptionadsorption method. The modified activated carbon showed high selectivity for separating CH 4 +CO 2 gas mixtures, compared with other methods to modify activated carbon given in the literature. The separation factor was 4.75 times higher than that for the fresh activated-carbon system, and the separation performance of the activated carbon increased with increasing amount of mIm. The addition of glycol showed greater potential to enhance the selectivity of the activated carbon than ethanol. A recycling test verified the stability of the modified activated carbon for CH 4 +CO 2 gas mixture separation.

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Computational Study on the Influences of Framework Charges on CO₂ Uptake in Metal−Organic Frameworks

Cited by 76 publications

References 32 publications

Molecular Simulation Studies of Separation of CO₂/N₂, CO₂/CH₄, and CH₄/N₂ by ZIFs

Molecular Simulation Studies of Separation of CO₂/N₂, CO₂/CH₄, and CH₄/N₂ by ZIFs

Accurate Ab Initio-Based Force Field for Predictive CO₂ Uptake Simulations in MOFs and ZIFs: Development and Applications for MTV-MOFs

Separation of Methane and Carbon Dioxide Gas Mixtures Using Activated Carbon Modified with 2‐Methylimidazole

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Computational Study on the Influences of Framework Charges on CO2 Uptake in Metal−Organic Frameworks

Cited by 76 publications

References 32 publications

Molecular Simulation Studies of Separation of CO2/N2, CO2/CH4, and CH4/N2 by ZIFs

Molecular Simulation Studies of Separation of CO2/N2, CO2/CH4, and CH4/N2 by ZIFs

Accurate Ab Initio-Based Force Field for Predictive CO2 Uptake Simulations in MOFs and ZIFs: Development and Applications for MTV-MOFs

Separation of Methane and Carbon Dioxide Gas Mixtures Using Activated Carbon Modified with 2‐Methylimidazole

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Computational Study on the Influences of Framework Charges on CO₂ Uptake in Metal−Organic Frameworks

Molecular Simulation Studies of Separation of CO₂/N₂, CO₂/CH₄, and CH₄/N₂ by ZIFs

Molecular Simulation Studies of Separation of CO₂/N₂, CO₂/CH₄, and CH₄/N₂ by ZIFs

Accurate Ab Initio-Based Force Field for Predictive CO₂ Uptake Simulations in MOFs and ZIFs: Development and Applications for MTV-MOFs