Journal article
Fluorinated Carbide-Derived Carbon: More Hydrophilic, Yet Apparently More Hydrophobic
Journal of the American Chemical Society, v 137(18), pp 5969-5979
13 May 2015
PMID: 25909685
Abstract
We explore the effect of fluorine doping on hydrophobicity of nanoporous silicon carbide-derived carbon (SiCDC), and investigate the underlying barriers for adsorption and diffusion Of water vapor and CO2 in the fluorinated and nonfluorinated structures: We develop atomistic models of fluorine-doped SiCDC at three different levels of fluorination, based on a hybrid reverse Monte Carlo constructed model of SiCDC, and develop a novel fir-principles force field for the simulation of adsorption and transport of water and CO2 in the fluorine-doped carbon materials. We demonstrate an apparent dual effect of fluorination, showing that while fluorination generates more hydrophilic carbon surfaces, they actually act as more hydrophobic structures due to enhanced energy barriers in the disordered network of micropoous carbon. While an increase in adsorption energy and in water uptake is seen for fluorine-doped carbon, large internal free energy barriers as well as the results of MD Simulations demonstrate that the increased adsorption is kinetically limited and not experimentally observable on practical time scales. We show that an increase in apparent hydrophobicity due to fluorination is mediated by larger free energy barriers arising from stronger binding of fluid molecules inside the pore network, as opposed to repulsion or steric hindrance to the diffusion of molecules through narrow pore entries. For carbon dioxide, adsorption enthalpies and activation energy barriers are both decreased on fluorination, indicating weakened solid fluid binding energies in the fluorinated systems.
Metrics
Details
- Title
- Fluorinated Carbide-Derived Carbon: More Hydrophilic, Yet Apparently More Hydrophobic
- Creators
- Amir H. Farmahini - The University of QueenslandDavid S. Sholl - Georgia Institute of TechnologySuresh K. Bhatia - The University of QueenslandEnergy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
- Publication Details
- Journal of the American Chemical Society, v 137(18), pp 5969-5979
- Publisher
- American Chemical Society; Washington, DC
- Number of pages
- 11
- Grant note
- Australian Government - National Computational Merit Allocation Scheme; Australian Government PACE (A Partnership for an Advanced Computing Environment) at the Georgia Institute of Technology, USA University of Queensland DE-SC0012577 / UNCAGE-ME, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences; United States Department of Energy (DOE) Australian Research Council (ARC); Australian Research Council
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Microbiology and Immunology
- Web of Science ID
- WOS:000354910500023
- Scopus ID
- 2-s2.0-84929376724
- Other Identifier
- 991021229906004721
InCites Highlights
Data related to this publication, from InCites Benchmarking & Analytics tool:
- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Chemistry, Multidisciplinary