Molecular Modeling as an Enabling Tool in Advanced Material Research
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1 Molecular Modeling as an Enabling Tool in Advanced Material Research Luke E. K. Achenie, Professor Virginia Polytechnic Institute and State University Chemical Engineering Department NSF (US/China) Workshop March
2 Outline Molecular Modeling Process Flexibility & Design Computational Science Oral Drug Delivery Membrane/CVD Research 2
3 With Oyama Group Molecular Dynamics Study (Hybrid Inorganic / Organic membranes) Membrane separation -- wide use in natural gas processing inorganic membrane Selective layer (silica, palladium) Intermediate layer (alumina) Support (alumina, stainless steel) 3
4 Hybrid Inorganic-Organic Membrane (exploit the reactivity of the Si-OR bonds) Prepared by high-temperature thermal PTES decomposition of organic precursors Polymer 4 Phenyltriethoxysilane Other derivatives:tetraethyl orthosilicate (TEOS)
5 Experimental data (need high P & S) STL-873-II At 373 K Selectivity: 19 S. Ted Oyama et al., Hybrid organic-inorganic gas separation membranes, US patent 7,938,894.,2011 May 10 5
6 Two Specific Aims 1. Construct Inorganic/Organic Membrane by MD 2. Simulate Separation of CO 2 /CH 4 by MD 6
7 AIM1-- Membrane Structure: Pore Creation and Insertion of Phenyl Groups - Zhenxing Wang, Luke E.K. Achenie, Sheima Jativ Khativa and S. Ted Oyama, Simulation study of carbon dioxide and methane gas permeation in hybrid organic-inorganic membrane, Journal of Membrane Science., 387/388, 30 39, # Å # Å # Å # Å 7 #1-1 #2-1 #3-2 #4-2
8 AIM 1 Phenyl Group & Partial Charge Effects Initial MD CO 2 (mol m -2 s -1 Pa -1 ) CH 4 (mol m -2 s -1 Pa -1 ) Selectivity No Phenyl Groups No Charge 7Phenyl Groups No Charge 7 Phenyl Groups Partial Charge
9 AIM 2: Gas Permeation P=2 MPa T=373 K NVT & NPT Dreiding force field Gas region 54 Å 9 - Zhenxing Wang, Luke E.K. Achenie, Sheima Jativ Khativa and S. Ted Oyama, Simulation study of carbon dioxide and methane gas permeation in hybrid organic-inorganic membrane, Journal of Membrane Science., 387/388, 30 39, 2012.
10 MD Simulation -- Gu, Yunfeng, Vaezian, Bita, Jatib Khatib, Sheima, Oyama, S. Ted, Wang, Zhenxing and Achenie, Luke, Hybrid H2-Selective Membranes Prepared by Chemical Vapor Deposition, Separation Science and Technology. 47(12), , Zhenxing Wang, Luke E.K. Achenie, Sheima Jativ Khativa and S. Ted Oyama, Simulation study of carbon dioxide and methane gas permeation in hybrid organic-inorganic membrane, Journal of Membrane Science., 387/388, 30 39, 2012.
11 Results of models without phenyl group Molecular dynamics study CO 2 permeance (mol m -2 s -1 Pa -1 ) CH 4 permeance (mol m -2 s -1 Pa -1 ) selectivity
12 Permeance of models with phenyl group Molecular dynamics study # Ph Grps O CO 2 permeance (mol m -2 s -1 Pa -1 ) CH 4 permeance (mol m -2 s -1 Pa -1 ) selectivity O S S S S Compare with Selectivity of 19 from Expts.
13 13 2 nd Modeling Approach Mixed Mechanisms
14 Mixed Mechanism Diffusion Model Micro-structure # 2 Micro-structure # 1 -- Zhenxing Wang, Luke E.K. Achenie, Sheima J. Khatib, and S. Ted Oyama (2013), Mixed mechanism model for permeation of gases in hybrid inorganic-organic membranes, Ind. Eng. Chem. Res., 52, ,
15 Some Results -- Zhenxing Wang, Luke E.K. Achenie, Sheima J. Khatib, and S. Ted Oyama (2013), Mixed mechanism model for permeation of gases in hybrid inorganic-organic membranes, Ind. Eng. Chem. Res., 52, ,
16 Zinc Sulfide Multi-Scale modeling of chemical vapor deposition processes Application: Used in the semiconductor industry to produce thin films on wafer substrate Reflective window Laser dooms Nano sensors Blue light diodes Luminescent displays Infra-red devices(anti reflection coating) T, Matsuoka, A. Ohki, T. Ohno, and Y.Kawaguchi, J. Cryst. Growth 138, 727, 1994.
17 CVD of Zinc Sulfide Gas phase reaction 2 2 Surface reactions ZnS( g) ZnS( s) Zn( g) H S ZnS( g) H ( g) H 2 S+Zn+Ar Substrate Outflow 17
18 Gas Phase reaction mechanism (ZnS) via DFT Molecular Modeling 18
19 Pathway selection and Deposition rate Zinc Sulfide concentration mol/m3 Deposition rate ( mm/day)[1] Sharifi, Y. and Achenie, L.E.K., Using Density Functional Theory to Postulate a Mechanism for Zinc Sulfide Formation in a CVD Reactor, Journal of Crystal Growth, 307, , Fang Z. et al, J of Crystal Growth, (2002)
20 Effect of substrate geometry on deposition rate Sharifi, Y. and Achenie, L.E.K. Effect of substrate geometry on deposition rate in CVD, Journal of Crystal Growth, 304, ,
21 Uniform Deposition Shape Optimization Sharifi, Y. and Achenie, L.E.K. Effect of substrate geometry on deposition rate in CVD, Journal of Crystal Growth, 304, ,
22 Cluster formation in Zinc Sulfide CVD Cause: 1. High temperature (973K) 2. Highly reactive precursors Disadvantages: 1. Particle settlement(gravity) 2. Outflow of particles 3. Impurity and defects [1]. 4. Inefficient Use of precursors Control the cluster formation [2]: 1. Mechanism 2. Dynamics What is the morphology of these particles? 22 [1] Wear 255 (2003) [2] Journal of Crystal Growth 208 (2000)
23 Particle size and distribution -- Sharifi, Y. and Achenie, L.E.K., Particle Dynamics in a CVD Reactor: A Multiscale Approach, Ind. Eng. Chem. Res., 48(13), ,
24 Summary Molecular Modeling as an Enabling Tool in Advanced Material Research
25 Acknowledgements: Funding from NSF, DOE Graduate Students Thank You!! 25
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