caa a22 4500 463170474 CHVBK 20180406164811.0 cr unu---uuuuu 170326e20071201xx s 000 0 eng 10.1007/s10450-007-9034-4 doi (NATIONALLICENCE)springer-10.1007/s10450-007-9034-4 Argon and krypton adsorption on templated mesoporous silicas: molecular simulation and experiment [Elektronische Daten] [Francisco Hung, Supriyo Bhattacharya, Benoit Coasne, Matthias Thommes, Keith Gubbins] In this work we report molecular simulation results for argon and krypton adsorption on atomistic models of templated mesoporous silica materials. These models add atomistic levels of detail to mesoscale representations of these porous materials, which were originally generated from lattice Monte Carlo simulations mimicking the synthesis process of templated mesoporous silicas. We generate our atomistic pore models by carving out of a silica block a ‘mathematically-smooth' representation of the pores from lattice MC simulations. Following that procedure, we obtain a model material with mean mesopore and micropore diameters of 5.4 nm and 1.1 nm, respectively (model A). Two additional model materials were considered: one with no microporosity, and with mesopores similar to those of model A (model B), and a regular cylindrical pore (model C). Simulation results for Ar and Kr adsorption on these model materials at 77 K and 87 K shows that model A provides the best agreement with experimental data; however, our results suggest that fine-tuning the microporosity and/or the surface chemistry (i.e., by decreasing the density of OH groups at the pore surface) of model A can lead to better agreement with experiments. The filling of the mesopores in model materials A and B proceeded via a classical capillary condensation mechanism, where the pores fill at slightly different pressures. This observation contrasts with what was observed in our previous study (Coasne, et al. in Langmuir 22:194-202, 2006), where we considered atomistic silica mesopores with an important degree of surface roughness at length scales below 10 Å, for which we observed a quasi-continuous mesopore filling involving intermediate phases with liquid-like "bridges” and gas-like regions. These results suggest that pore surface roughness, and other morphological features such as constrictions, play an important role in the mechanism of adsorption and filling of the mesopores. Springer Science+Business Media, LLC, 2007 Templated mesoporous silica materials nationallicence MCM-41 nationallicence SBA-15 nationallicence Gas adsorption nationallicence Molecular simulation nationallicence Monte Carlo nationallicence Hung Francisco Department of Chemical and Biological Engineering, University of Wisconsin, 53706-1691, Madison, WI, USA aut Bhattacharya Supriyo Center for High Performance Simulation and Department of Chemical and Biomolecular Engineering, North Carolina State University, 27695-7905, Raleigh, NC, USA aut Coasne Benoit Institut Charles Gerhardt Montpellier, CNRS (UMR 56253), University Montpellier 2, and ENSCM, cedex 5, 34095, Montpellier, France aut Thommes Matthias Quantachrome Instruments, 33426, Boynton Beach, FL, USA aut Gubbins Keith Center for High Performance Simulation and Department of Chemical and Biomolecular Engineering, North Carolina State University, 27695-7905, Raleigh, NC, USA aut Adsorption Springer US; http://www.springer-ny.com 13/5-6(2007-12-01), 425-437 0929-5607 13:5-6<425 2007 13 10450 https://doi.org/10.1007/s10450-007-9034-4 text/html Onlinezugriff via DOI 1 research-article jats NATIONALLICENCE 856 40 https://doi.org/10.1007/s10450-007-9034-4 text/html Onlinezugriff via DOI NATIONALLICENCE 700 1- Hung Francisco Department of Chemical and Biological Engineering, University of Wisconsin, 53706-1691, Madison, WI, USA aut NATIONALLICENCE 700 1- Bhattacharya Supriyo Center for High Performance Simulation and Department of Chemical and Biomolecular Engineering, North Carolina State University, 27695-7905, Raleigh, NC, USA aut NATIONALLICENCE 700 1- Coasne Benoit Institut Charles Gerhardt Montpellier, CNRS (UMR 56253), University Montpellier 2, and ENSCM, cedex 5, 34095, Montpellier, France aut NATIONALLICENCE 700 1- Thommes Matthias Quantachrome Instruments, 33426, Boynton Beach, FL, USA aut NATIONALLICENCE 700 1- Gubbins Keith Center for High Performance Simulation and Department of Chemical and Biomolecular Engineering, North Carolina State University, 27695-7905, Raleigh, NC, USA aut NATIONALLICENCE 773 0- Adsorption Springer US; http://www.springer-ny.com 13/5-6(2007-12-01), 425-437 0929-5607 13:5-6<425 2007 13 10450 Metadata rights reserved Springer special CC-BY-NC licence nationallicence BK010053 XK010053 XK010000 NATIONALLICENCE NATIONALLICENCE NL-springer