Alkylsilane-Functionalized Microporous and Mesoporous Materials: Molecular Simulation and Experimental Analysis of Gas Adsorption

Solid sorbents are considered as a potentially less-energy-intensive alternative to the use of liquids for the removal and separation of liquid and gaseous fluids. The control of the surface characteristics of porous inorganic materials via the deposition of an organic layer is of great interest for tailoring the properties of the sorbent. For instance, organic functionalization of traditional solid sorbents (micro- and mesoporous silica and silicates) allows tuning their surface properties, such as hydrophilicity or hydrophobicity and surface reactivity. However, the underlying mechanism of the sorption process in highly complex organic functionalized materials is not yet fully understood. This incomplete understanding limits the possibilities of designing optimal adsorbents for different applications increasing the interest in performing complementary experimental-simulation studies. In this work, the adsorption of N2 in alkylsilane-modified disordered mesoporous silica (silica gel 40) and crystalline a...

[1]  A. Fadeev,et al.  Thermal stability of organic monolayers chemically grafted to minerals. , 2005, Journal of colloid and interface science.

[2]  P. Llewellyn,et al.  Adsorption mechanism of carbon dioxide in faujasites: grand canonical monte carlo simulations and microcalorimetry measurements. , 2005, The journal of physical chemistry. B.

[3]  T. Düren,et al.  Influence of Surface Groups on the Diffusion of Gases in MCM-41: A Molecular Dynamics Study , 2011 .

[4]  T. W. Żerda,et al.  Properties of liquid acetone in silica pores: Molecular dynamics simulation , 1996 .

[5]  A. Cheetham,et al.  Silanol chemistry in siliceous faujasite , 1992 .

[6]  W. Tong,et al.  A review of zeolite-like porous materials , 2000 .

[7]  Ying Zhang,et al.  Novel synthesis and molecularly scaled surface hydrophobicity control of colloidal mesoporous silica , 2011 .

[8]  K. Kaneko.  Determination of pore size and pore size distribution1. Adsorbents and catalysts , 1994 .

[9]  J. Ilja Siepmann,et al.  Vapor–liquid equilibria of mixtures containing alkanes, carbon dioxide, and nitrogen , 2001 .

[10]  B. K. Mishra,et al.  Organically modified silica: synthesis and applications due to its surface interaction with organic molecules. , 2008, Advances in colloid and interface science.

[11]  T. Düren,et al.  Effect of Surface Group Functionalization on the CO2/N2 Separation Properties of MCM-41: A Grand-Canonical Monte Carlo Simulation Study , 2010 .

[12]  L. Vega,et al.  Microporous carbon adsorbents with high CO2 capacities for industrial applications. , 2011, Physical chemistry chemical physics : PCCP.

[13]  V. Rotello,et al.  Monolayer coated gold nanoparticles for delivery applications. , 2012, Advanced drug delivery reviews.

[14]  N. L. Allinger,et al.  Molecular mechanics (MM2) calculations on siloxanes , 1989 .

[15]  N. Seaton,et al.  Development and Validation of Pore Structure Models for Adsorption in Activated Carbons , 1999 .

[16]  C. Domingo,et al.  Preparation of silane-coated TiO2 nanoparticles in supercritical CO2. , 2009, Journal of colloid and interface science.

[17]  P. Wright,et al.  Design of hybrid organic/inorganic adsorbents based on periodic mesoporous silica , 2006 .

[18]  H. Takaba,et al.  Molecular dynamics calculations of CO2/N2 mixture through the NaY type zeolite membrane , 2001 .

[19]  K. Gubbins,et al.  Nitrogen adsorption in carbon aerogels: A molecular simulation study , 2002 .

[20]  K. Raghavan,et al.  Adsorption and diffusion of a Lennard‐Jones vapor in microporous silica , 1990 .

[21]  Randall Q. Snurr,et al.  Prediction of adsorption of aromatic hydrocarbons in silicalite from grand canonical Monte Carlo simulations with biased insertions , 1993 .

[22]  P. Wright,et al.  Generation of atomistic models of periodic mesoporous silica by kinetic Monte Carlo simulation of the synthesis of the material. , 2006, The journal of physical chemistry. B.

[23]  Concepción Domingo,et al.  Preparation and Characterization of Surface Silanized TiO2 Nanoparticles under Compressed CO2: Reaction Kinetics , 2009 .

[24]  T. J. McCarthy,et al.  Chemical modification of chromium oxide surfaces using organosilanes. , 2009, Journal of colloid and interface science.

[25]  Lourdes F. Vega,et al.  THERMODYNAMIC BEHAVIOUR OF HOMONUCLEAR AND HETERONUCLEAR LENNARD-JONES CHAINS WITH ASSOCIATION SITES FROM SIMULATION AND THEORY , 1997 .

[26]  Karen Wilson,et al.  Interdependent lateral interactions, hydrophobicity and acid strength and their influence on the catalytic activity of nanoporous sulfonic acid silicas , 2010 .

[27]  Lourdes F. Vega,et al.  Understanding CO2 Capture in Amine-Functionalized MCM-41 by Molecular Simulation , 2012 .

[28]  L. Vega,et al.  Optimization of the separation of sulfur hexafluoride and nitrogen by selective adsorption using monte carlo simulations , 2011 .

[29]  T. Takei,et al.  Porous properties of silylated mesoporous silica and its hydrogen adsorption , 2007 .

[30]  A. Navrotsky,et al.  High-silica zeolites: a relationship between energetics and internal surface areas , 2002 .

[31]  K. Raghavan,et al.  Transport of an adsorbing vapour in a model silica system , 1991 .

[32]  A. Frischknecht,et al.  Using arbitrary trial distributions to improve intramolecular sampling in configurational-bias Monte Carlo , 2006 .

[33]  J. MacElroy.  Molecular simulation of the kinetic selectivity of a model silica system , 2002 .

[34]  A. Fadeev,et al.  Self-assembled monolayers supported on TiO2: Comparison of C18H37SiX3 (X = H, Cl, OCH3), C18H37Si(CH3)2Cl, and C18H37PO(OH)2 , 2002 .

[35]  Lourdes F. Vega,et al.  Sorption of tryalkoxysilane in low-cost porous silicates using a supercritical CO2 method , 2012 .

[36]  J. Ilja Siepmann,et al.  Novel Configurational-Bias Monte Carlo Method for Branched Molecules. Transferable Potentials for Phase Equilibria. 2. United-Atom Description of Branched Alkanes , 1999 .

[37]  K. Sing.  Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984) , 1985 .

[38]  Parveen Kumar,et al.  Periodic mesoporous organic–inorganic hybrid materials: Applications in membrane separations and adsorption , 2010 .