TY  - JOUR
A1  - Tsendra, Oksana
A1  - Scott, Andrea Michalkova
A1  - Gorb, Leonid
A1  - Boese, Adrian Daniel
A1  - Hill, Frances C.
A1  - Ilchenko, Mykola M.
A1  - Leszczynska, Danuta
A1  - Leszczynski, Jerzy
T1  - Adsorption of Nitrogen-Containing Compounds on the (100) alpha-Quartz Surface: Ab Initio Cluster Approach
JF  - The journal of physical chemistry : C, Nanomaterials and interfaces
N2  - A cluster approach extended to the ONIOM methodology has been applied using several density functionals and Moller-Plesset perturbation theory (MP2) to simulate the adsorption of selected nitrogen-containing compounds [NCCs, 2,4,6-trinitrotoluene (TNT), 2,4-dinitrotoluene (DNT), 2,4-dinitroanisole (DNAN), and 3-nitro-1,2,4-triazole-5-one (NTO)] on the hydroxyated (100) surface of a-quartz. The structural properties were calculated using the M06-2X functional and 6-31G(d,p) basis set. The M06-2X-D3, PBE-D3, and MP2 methods were used to calculate the adsorption energies. Results have been compared with the data from other studies of adsorption of compounds of similar nature on silica. Effect of deformation of the silica surface and adsorbates on the binding energy values was also studied. The atoms in molecules (AIM) analysis was employed to characterize the adsorbate-adsorbent binding and to calculate the bond energies. The silica surface shows different sorption affinity toward the chemicals considered depending on their electronic structure. All target NCCs are physisorbed on the modeled silica surface. Adsorption occurs due to the formation of multiple hydrogen bonds between the functional groups of NCCs and surface silanol groups. Parallel orientation of NCCs interacting with the silica surface was found to be favorable when compared with perpendicularly oriented NCCs. NTO was found to be the most strongly adsorbed on the silica surface among all of the considered compounds. Dispersion correction was shown to play an important role in the DFT calculations of the adsorption energies of silica-NCC systems.
Y1  - 2014
U6  - https://doi.org/10.1021/jp406827h
SN  - 1932-7447
VL  - 118
IS  - 6
SP  - 3023
EP  - 3034
PB  - American Chemical Society
CY  - Washington
ER  -