Dataset Information

A computational study of CH4 storage in porous framework materials with metalated linkers: connecting the atomistic character of CH4 binding sites to usable capacity.

ABSTRACT: To store natural gas (NG) inexpensively at adequate densities for use as a fuel in the transportation sector, new porous materials are being developed. This work uses computational methods to explore strategies for improving the usable methane storage capacity of adsorbents, including metal-organic frameworks (MOFs), that feature open-metal sites incorporated into their structure by postsynthetic modification. The adsorption of CH4 on several open-metal sites is studied by calculating geometries and adsorption energies and analyzing the relevant interaction factors. Approximate site-specific adsorption isotherms are obtained, and the open-metal site contribution to the overall CH4 usable capacity is evaluated. It is found that sufficient ionic character is required, as exemplified by the strong CH4 affinities of 2,2'-bipyridine-CaCl2 and Mg, Ca-catecholate. In addition, it is found that the capacity of a single metal site depends not only on its affinity but also on its geometry, where trigonal or "bent" low-coordinate exposed sites can accommodate three or four methane molecules, as exemplified by Ca-decorated nitrilotriacetic acid. The effect of residual solvent molecules at the open-metal site is also explored, with some positive conclusions. Not only can residual solvent stabilize the open-metal site, surprisingly, solvent molecules do not necessarily reduce CH4 affinity, but can contribute to increased usable capacity by modifying adsorption interactions.

SUBMITTER: Tsivion E

PROVIDER: S-EPMC6016331 | biostudies-literature | 2016 Jul

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

A computational study of CH4 storage in porous framework materials with metalated linkers: connecting the atomistic character of CH4 binding sites to usable capacity.

Tsivion Ehud E Mason Jarad A JA Gonzalez Miguel I MI Long Jeffrey R JR Head-Gordon Martin M

Chemical science 20160329 7

To store natural gas (NG) inexpensively at adequate densities for use as a fuel in the transportation sector, new porous materials are being developed. This work uses computational methods to explore strategies for improving the usable methane storage capacity of adsorbents, including metal-organic frameworks (MOFs), that feature open-metal sites incorporated into their structure by postsynthetic modification. The adsorption of CH4 on several open-metal sites is studied by calculating ...[more]

PMID: 30155097

Similar Datasets

Project description:The separation of CO2/CH4 using porous carbon can be increased by the presence of a functional group of nitrogen on the carbon surface. This study explores the potential of porous carbon derived from the palm kernel shell (C-PKS) impregnated with a deep eutectic solvent (DES), which is one of the chemicals containing a nitrogen element. The DES was composed of a quaternary ammonium salt of choline chloride (ChCl) and a hydrogen bond donor of alcohol. Three alcohols of 1-butanol (-ol), ethylene glycol (-diol), and glycerol (-triol) were employed to study the effects of a number of hydroxyl groups in the separation performance. The research steps included (i) the preparation of DES-impregnated porous carbon synthesized from the palm kernel shell (DES/C-PKS), (ii) characterization of the material, and (ii) a separation test of CO2/CH4 with a breakthrough system. Materials were characterized using scanning electron microscopy (SEM) combined with energy-dispersive X-ray spectroscopy (EDX), N2-sorption analysis, and Fourier transform infrared (FTIR) spectroscopy. SEM images showed a significant morphological difference of pristine carbon and DES/C-PKS. There was a significant decrease in the range of 67-73% of a specific surface area with respect to pristine carbon, having initially 800 m2/g. However, the N element on the carbon surface increased after impregnation treatment, which was shown from the intensity of the FTIR graphs and EDX analysis. Adsorption isotherm revealed that DES/C-PKS could enhance up to 1.6 times the adsorption capacity of CO2 at 1 atm and 30 °C while increasing the selectivity of CO2/CH4 up to 125%. The breakthrough experiment showed that all DES/C-PKS materials displayed a better performance for the separation of CO2/CH4, indicated by a longer breakthrough time and enhancement of CO2 uptake. The best separation performance was achieved by DES/C-PKS using glycerol as a hydrogen bond donor with 15.4 mg/g of CO2 uptake or equivalent to 95% enhancement of the uptake capacity compared to pristine porous carbon. Also, the cycling test revealed that DES/C-PKS can be used repetitively, which further highlights the efficiency of the material for the separation of CO2/CH4.

Dataset Information

A computational study of CH4 storage in porous framework materials with metalated linkers: connecting the atomistic character of CH4 binding sites to usable capacity.

Publications

A computational study of CH<sub>4</sub> storage in porous framework materials with metalated linkers: connecting the atomistic character of CH<sub>4</sub> binding sites to usable capacity.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets