Computational investigation on CO2 adsorption in titanium carbide-derived carbons with residual titanium

Abstract

This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. AbstractWe develop a new approach for modeling titanium carbide derived-carbon (TiC-CDC) systems with residual titanium by the generation of modified atomistic structures based on a silicon carbide derived-carbon (SiC-CDC) model and the application of weighted combinations of these structures.In our approach, the original SiC-CDC structure is modified by (i) removing carbon, (ii) adding carbon and (iii) adding titanium. The new atomic scale carbide-derived carbon (CDC) structures are investigated using classical molecular dynamics simulations, and their pure CO 2 adsorption isotherms are calculated using grand canonical Monte Carlo simulations. The system of TiC-CDC with residual titanium is modeled as weighted combinations of pure carbon CDC structures, CDC structures with titanium and a TiC crystalline structure. Our modeling is able to produce both M A N U S C R I P T A C C E P T E D ACCEPTED MANUSCRIPTstructural properties and adsorption isotherms in accordance with experimental data. The fraction of different models in the systems successfully reflects the structural differences in various experimental TiC-CDC samples. The modeling also suggests that in partially etched TiC-CDC systems, the titanium that may be accessible to CO 2 gas at the transitional interface may provide significant interaction sites for CO 2 and may lead to more efficient overall gas adsorption.

Molecular Modeling of Microporous Structures of Carbide-Derived Carbon-Based Supercapacitors

“…In a similar manner, Zhang et al. have successfully performed computational studies on TiC-CDC material based on SiC-derived structures …”

“…In a similar manner, Zhang et al have successfully performed computational studies on TiC-CDC material based on SiC-derived structures. 45 Over 200 polymorphs of silicon carbide are known. 4H-SiC belongs to the technologically most important ones and is used in our work as initial structure for modeling CDC-like structures.…”

Molecular Simulation of Capture of Sulfur-Containing Gases by Porous Aromatic Frameworks

“…Note that most actual PAF materials have degrees of long-range disorder, ,,, whereas the models we have used are for entirely crystalline materials. Although atomistic methods can be applied to partially ordered or amorphous materials, or even more complicated heterogeneous disordered systems when appropriate structural models are available, ,− generation of accurate models of this kind is challenging and is beyond the scope of this work. It seems unlikely that the overall trends identified in our calculations with crystalline models would change substantially if a thorough assessment of disorder effects in PAFs was made.…”

Graphene–Titanium Interfaces from Molecular Dynamics Simulations

“…We are aware of only one MD study of fullerenes decorated with small titanium clusters that used a classical Lennard-Jones potential 51 and one recent study of Ti clusters on carbide-derived carbon. 52 This study used the third generation of the charge-optimized many-body (COMB3) potential, 53 recently parameterized to simulate Ti−C−O−H multicomponent systems. 54 Here, we report the first classical MD study of G−Ti interfaces, using the COMB3 potential.…”