Witman, M;
Ling, S;
Gładysiak, A;
Stylianou, KC;
Smit, B;
Slater, B;
Haranczyk, M;
(2017)
Rational Design of a Low-Cost, High-Performance Metal-Organic Framework for Hydrogen Storage and Carbon Capture.
The Journal of Physical Chemistry C
, 121
(2)
pp. 1171-1181.
10.1021/acs.jpcc.6b10363.
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Abstract
We present the in silico design of a MOF-74 analogue, hereon known as M2(DHFUMA) [M = Mg, Fe, Co, Ni, Zn], with enhanced small-molecule adsorption properties over the original M2(DOBDC) series. Constructed from 2,3-dihydroxyfumarate (DHFUMA), an aliphatic ligand which is smaller than the aromatic 2,5-dioxidobenzene-1,4-dicarboxylate (DOBDC), the M2(DHFUMA) framework has a reduced channel diameter, resulting in higher volumetric density of open metal sites and significantly improved volumetric hydrogen (H2) storage potential. Furthermore, the reduced distance between two adjacent open metal sites in the pore channel leads to a CO2 binding mode of one molecule per two adjacent metals with markedly stronger binding energetics. Through dispersion-corrected density functional theory (DFT) calculations of guest–framework interactions and classical simulation of the adsorption behavior of binary CO2:H2O mixtures, we theoretically predict the M2(DHFUMA) series as an improved alternative for carbon capture over the M2(DOBDC) series when adsorbing from wet flue gas streams. The improved CO2 uptake and humidity tolerance in our simulations is tunable based upon metal selection and adsorption temperature which, combined with the significantly reduced ligand expense, elevates this material’s potential for CO2 capture and H2 storage. The dynamical and elastic stabilities of Mg2(DHFUMA) were verified by hybrid DFT calculations, demonstrating its significant potential for experimental synthesis.
| Type: | Article |
|---|---|
| Title: | Rational Design of a Low-Cost, High-Performance Metal-Organic Framework for Hydrogen Storage and Carbon Capture |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.jpcc.6b10363 |
| Publisher version: | http://dx.doi.org/10.1021/acs.jpcc.6b10363 |
| Language: | English |
| Additional information: | Copyright © 2016 American Chemical Society. This is an open access article published under an ACS AuthorChoice License - http://pubs.acs.org/page/policy/authorchoice_termsofuse.html - which permits copying and redistribution of the article or any adaptations for non-commercial purposes. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/1536745 |
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