Modeling the Structural Heterogeneity of Vicinal Silanols and Its Effects on TiCl 4 Grafting onto Amorphous Silica

Khan, Salman A.; Godahewa, Sahan M.; Wimalasiri, Pubudu N.; Thompson, Ward H.; Scott, Susannah L.; Peters, Baron

doi:10.1021/acs.chemmater.1c04016

Modeling the Structural Heterogeneity of Vicinal Silanols and Its Effects on TiCl ₄ Grafting onto Amorphous Silica

Journal Article · 24 April 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c04016· OSTI ID:1977795

^[1]; Godahewa, Sahan M. ^[2]; Wimalasiri, Pubudu N. ^[2]; ^[2]; ^[3]; ^[4]

Department of Chemical Engineering, University of California, Santa Barbara, California 93106, United States
Department of Chemistry, University of Kansas, Lawrence, Kansas 66045, United States
Department of Chemical Engineering, University of California, Santa Barbara, California 93106, United States; Department of Chemistry & Biochemistry, University of California, Santa Barbara, California 93106, United States
Department of Chemical & Biomolecular Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States; Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States

Not provided.

Research Organization:: Univ. of California, Santa Barbara, CA (United States); Univ. of Kansas, Lawrence, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: FG02-03ER15467; SC0019488

OSTI ID:: 1977795

Journal Information:: Chemistry of Materials, Vol. 34, Issue 9; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

References (68)

A new titanium-silica catalyst for the epoxidation of alkenes Cativiela, Carlos; Fraile, JoséM.; García, JoséI. Journal of Molecular Catalysis A: Chemical, Vol. 112, Issue 2 https://doi.org/10.1016/1381-1169(96)00131-8	journal	October 1996
A Well-Defined, Silica-Supported Tungsten Imido Alkylidene Olefin Metathesis Catalyst Rhers, Bouchra; Salameh, Alain; Baudouin, Anne Organometallics, Vol. 25, Issue 15 https://doi.org/10.1021/om060279d	journal	July 2006
Ultrathin (<4 nm) SiO2 and Si–O–N gate dielectric layers for silicon microelectronics: Understanding the processing, structure, and physical and electrical limits Green, M. L.; Gusev, E. P.; Degraeve, R. Journal of Applied Physics, Vol. 90, Issue 5 https://doi.org/10.1063/1.1385803	journal	September 2001
SiO2 surface passivation layers – a key technology for silicon solar cells Glunz, Stefan W.; Feldmann, Frank Solar Energy Materials and Solar Cells, Vol. 185 https://doi.org/10.1016/j.solmat.2018.04.029	journal	October 2018
Silica waveguides on silicon and their application to integrated-optic components Kawachi, Masao Optical and Quantum Electronics, Vol. 22, Issue 5 https://doi.org/10.1007/BF02113964	journal	September 1990
Silica, Hybrid Silica, Hydride Silica and Non-Silica Stationary Phases for Liquid Chromatography Borges, Endler M. Journal of Chromatographic Science, Vol. 53, Issue 4 https://doi.org/10.1093/chromsci/bmu090	journal	September 2014
Medium-range structural order in covalent amorphous solids Elliott, S. R. Nature, Vol. 354, Issue 6353 https://doi.org/10.1038/354445a0	journal	December 1991
Revealing hidden medium-range order in amorphous materials using topological data analysis Sørensen, Søren S.; Biscio, Christophe A. N.; Bauchy, Mathieu Science Advances, Vol. 6, Issue 37 https://doi.org/10.1126/sciadv.abc2320	journal	September 2020
Nearly free surface silanols are the critical molecular moieties that initiate the toxicity of silica particles Pavan, Cristina; Santalucia, Rosangela; Leinardi, Riccardo Proceedings of the National Academy of Sciences, Vol. 117, Issue 45 https://doi.org/10.1073/pnas.2008006117	journal	October 2020
The Fumed Silica Surface: A Study by NMR Liu, Changhua C.; Maciel, Gary E. Journal of the American Chemical Society, Vol. 118, Issue 21 https://doi.org/10.1021/ja954120w	journal	January 1996
Formation of Digallium Sites in the Reaction of Trimethylgallium with Silica Taha, Ziyad A.; Deguns, Eric W.; Chattopadhyay, Swarup Organometallics, Vol. 25, Issue 8 https://doi.org/10.1021/om051034o	journal	April 2006
Evidence for the Pairwise Disposition of Grafting Sites on Highly Dehydroxylated Silicas via Their Reactions with Ga(CH ₃ ) ₃ Fleischman, Samuel D.; Scott, Susannah L. Journal of the American Chemical Society, Vol. 133, Issue 13 https://doi.org/10.1021/ja108905p	journal	April 2011
Beyond Ordered Materials: Understanding Catalytic Sites on Amorphous Solids Goldsmith, Bryan R.; Peters, Baron; Johnson, J. Karl ACS Catalysis, Vol. 7, Issue 11 https://doi.org/10.1021/acscatal.7b01767	journal	October 2017
Catalysis by Design: Well-Defined Single-Site Heterogeneous Catalysts Pelletier, Jérémie D. A.; Basset, Jean-Marie Accounts of Chemical Research, Vol. 49, Issue 4 https://doi.org/10.1021/acs.accounts.5b00518	journal	March 2016
Design and engineering of multifunctional silica-supported cooperative catalysts Fernandes, Antony E.; Jonas, Alain M. Catalysis Today, Vol. 334 https://doi.org/10.1016/j.cattod.2018.11.040	journal	August 2019
Reactions of silica surfaces with hydrogen sequestering agents Kunawicz (née Murray), J.; Jones, P.; Hockey, J. A. Trans. Faraday Soc., Vol. 67, Issue 0 https://doi.org/10.1039/TF9716700848	journal	January 1971
Dispersion and distribution of titanium species bound to silica from titanium tetrachloride Haukka, Suvi; Lakomaa, Eeva Liisa; Jylha, Olli Langmuir, Vol. 9, Issue 12 https://doi.org/10.1021/la00036a026	journal	December 1993
An IR and NMR study of the chemisorption of titanium tetrachloride on silica Haukka, Suvi; Lakomaa, Eeva Liisa; Root, Andrew The Journal of Physical Chemistry, Vol. 97, Issue 19 https://doi.org/10.1021/j100121a040	journal	May 1993
Thermal Restructuring of Silica-Grafted TiCl _x Species and Consequences for Epoxidation Catalysis Mania, Philipp; Verel, René; Jenny, Florian Chemistry - A European Journal, Vol. 19, Issue 30 https://doi.org/10.1002/chem.201300842	journal	June 2013
Theoretical Investigations of Heterogeneous Olefin Metathesis Catalysts Handzlik, Jaroslaw; Kurleto, Kamil Current Organic Chemistry, Vol. 17, Issue 22 https://doi.org/10.2174/13852728113179990119	journal	October 2013
Molecular models in ab initio studies of solids and surfaces: from ionic crystals and semiconductors to catalysts Sauer, Joachim Chemical Reviews, Vol. 89, Issue 1 https://doi.org/10.1021/cr00091a006	journal	January 1989
Effect of Siloxane Ring Strain and Cation Charge Density on the Formation of Coordinately Unsaturated Metal Sites on Silica: Insights from Density Functional Theory (DFT) Studies Das, Ujjal; Zhang, Guanghui; Hu, Bo ACS Catalysis, Vol. 5, Issue 12 https://doi.org/10.1021/acscatal.5b01699	journal	November 2015
High-resolution 29 Si CP/MAS solid state NMR spectroscopy and DFT investigation on the role of geminal and single silanols in grafting chromium species over Phillips Cr/silica catalyst Cheng, Ruihua; Liu, Xuee; Fang, Yuwei Applied Catalysis A: General, Vol. 543 https://doi.org/10.1016/j.apcata.2017.05.011	journal	August 2017
Grafting of Lanthanide Complexes on Silica Surfaces: A Theoretical Investigation Del Rosal, Iker; Gerber, Iann C.; Poteau, Romuald The Journal of Physical Chemistry A, Vol. 114, Issue 21 https://doi.org/10.1021/jp101495n	journal	June 2010
Atomic Layer Deposition of TiO₂ from TiI₄ and H₂O onto SiO₂ Surfaces: Ab Initio Calculations of the Initial Reaction Mechanisms Hu, Zheng; Turner, C. Heath Journal of the American Chemical Society, Vol. 129, Issue 13 https://doi.org/10.1021/ja066529z	journal	March 2007
Initial Surface Reactions of TiO₂ Atomic Layer Deposition onto SiO₂ Surfaces: Density Functional Theory Calculations Hu, Zheng; Turner, C. Heath The Journal of Physical Chemistry B, Vol. 110, Issue 16 https://doi.org/10.1021/jp060367b	journal	April 2006
DFT Studies of the Structure and Vibrational Spectra of Isolated Molybdena Species Supported on Silica Chempath, Shaji; Zhang, Yihua; Bell, Alexis T. The Journal of Physical Chemistry C, Vol. 111, Issue 3 https://doi.org/10.1021/jp064741j	journal	December 2006
Structure of Isolated Molybdenum(VI) and Molybdenum(IV) Oxide Species on Silica: Periodic and Cluster DFT Studies Handzlik, Jarosław; Ogonowski, Jan The Journal of Physical Chemistry C, Vol. 116, Issue 9 https://doi.org/10.1021/jp207385h	journal	February 2012
Application of the ONIOM (QM/QM) method in the study of molybdena–silica system active in olefin metathesis Handzlik, Jarosław International Journal of Quantum Chemistry, Vol. 107, Issue 11 https://doi.org/10.1002/qua.21397	journal	January 2007
Characterization of molybdenum monomeric oxide species supported on hydroxylated silica: a DFT study Guesmi, Hazar; Gryboś, Robert; Handzlik, Jarosław Phys. Chem. Chem. Phys., Vol. 16, Issue 34 https://doi.org/10.1039/C4CP02296C	journal	January 2014
Interaction between transition metals (Co, Ni, and Cu) systems and amorphous silica surfaces: A DFT investigation Gueddida, Saber; Lebègue, Sébastien; Badawi, Michael Applied Surface Science, Vol. 533 https://doi.org/10.1016/j.apsusc.2020.147422	journal	December 2020
Chromium Oxide Species Supported on Silica: A Representative Periodic DFT Model Guesmi, Hazar; Tielens, Frederik The Journal of Physical Chemistry C, Vol. 116, Issue 1 https://doi.org/10.1021/jp209680r	journal	December 2011
Toward the Atomic Scale Simulation of Intricate Acidic Aluminosilicate Catalysts Chizallet, Céline ACS Catalysis, Vol. 10, Issue 10 https://doi.org/10.1021/acscatal.0c01136	journal	April 2020
Brønsted acidity of amorphous silica–alumina: The molecular rules of proton transfer Leydier, Fabien; Chizallet, Céline; Chaumonnot, Alexandra Journal of Catalysis, Vol. 284, Issue 2 https://doi.org/10.1016/j.jcat.2011.08.015	journal	December 2011
Accurate Amorphous Silica Surface Models from First-Principles Thermodynamics of Surface Dehydroxylation Ewing, Christopher S.; Bhavsar, Saurabh; Veser, Götz Langmuir, Vol. 30, Issue 18 https://doi.org/10.1021/la500422p	journal	April 2014
Amorphous SiO ₂ surface models: energetics of the dehydroxylation process, strain, ab initio atomistic thermodynamics and IR spectroscopic signatures Comas-Vives, Aleix Physical Chemistry Chemical Physics, Vol. 18, Issue 10 https://doi.org/10.1039/C6CP00602G	journal	January 2016
Ab Initio Study of the Hydroxylated Surface of Amorphous Silica: A Representative Model Tielens, Frederik; Gervais, Christel; Lambert, Jean François Chemistry of Materials, Vol. 20, Issue 10 https://doi.org/10.1021/cm8001173	journal	May 2008
Imprinting isolated single iron atoms onto mesoporous silica by templating with metallosurfactants Berro, Y.; Gueddida, S.; Bouizi, Y. Journal of Colloid and Interface Science, Vol. 573 https://doi.org/10.1016/j.jcis.2020.03.095	journal	August 2020
Simulations of Ammonia Adsorption for the Characterization of Acid Sites in Metal-Doped Amorphous Silicates Jystad, Amy M.; Biancardi, Alessandro; Caricato, Marco The Journal of Physical Chemistry C, Vol. 121, Issue 40 https://doi.org/10.1021/acs.jpcc.7b08113	journal	September 2017
Computational Investigation of the Role of Active Site Heterogeneity for a Supported Organovanadium(III) Hydrogenation Catalyst Patel, Prajay; Wells, Robert H.; Kaphan, David M. ACS Catalysis, Vol. 11, Issue 12 https://doi.org/10.1021/acscatal.1c00688	journal	June 2021
Single-Molecule Kinetics of Styrene Hydrogenation on Silica-Supported Vanadium: The Role of Disorder for Single-Atom Catalysts Wells, Robert H.; An, Suming; Patel, Prajay The Journal of Physical Chemistry C, Vol. 125, Issue 37 https://doi.org/10.1021/acs.jpcc.1c04759	journal	September 2021
Site-averaged kinetics for catalysts on amorphous supports: an importance learning algorithm Vandervelden, Craig; Khan, Salman Ahmad; Scott, Susannah L. Reaction Chemistry & Engineering https://doi.org/10.1039/C9RE00356H	journal	January 2019
Importance learning estimator for the site-averaged turnover frequency of a disordered solid catalyst Vandervelden, Craig A.; Khan, Salman A.; Peters, Baron The Journal of Chemical Physics, Vol. 153, Issue 24 https://doi.org/10.1063/5.0037450	journal	December 2020
Nonhydrolytic Surface Synthesis of a Heterobimetallic V−Ti Alkoxide Complex on Silica Rice, Gordon L.; Scott, Susannah L. Chemistry of Materials, Vol. 10, Issue 2 https://doi.org/10.1021/cm9706199	journal	January 1998
Nature of ≡SiOCrO ₂ Cl and (≡SiO) ₂ CrO ₂ Sites Prepared by Grafting CrO ₂ Cl ₂ onto Silica Demmelmaier, Cori A.; White, Rosemary E.; van Bokhoven, Jeroen A. The Journal of Physical Chemistry C, Vol. 112, Issue 16 https://doi.org/10.1021/jp7119153	journal	April 2008
Long-range corrected hybrid density functionals with damped atom–atom dispersion corrections Chai, Jeng-Da; Head-Gordon, Martin Physical Chemistry Chemical Physics, Vol. 10, Issue 44 https://doi.org/10.1039/b810189b	journal	January 2008
The role of databases in support of computational chemistry calculations Feller, David Journal of Computational Chemistry, Vol. 17, Issue 13 https://doi.org/10.1002/(SICI)1096-987X(199610)17:13<1571::AID-JCC9>3.0.CO;2-P	journal	October 1996
Isolated catalyst sites on amorphous supports: A systematic algorithm for understanding heterogeneities in structure and reactivity Goldsmith, Bryan R.; Sanderson, Evan D.; Bean, Daniel The Journal of Chemical Physics, Vol. 138, Issue 20 https://doi.org/10.1063/1.4807384	journal	May 2013
Basis Set Exchange: A Community Database for Computational Sciences Schuchardt, Karen L.; Didier, Brett T.; Elsethagen, Todd Journal of Chemical Information and Modeling, Vol. 47, Issue 3 https://doi.org/10.1021/ci600510j	journal	March 2007
Optimization of Gaussian-type basis sets for local spin density functional calculations. Part I. Boron through neon, optimization technique and validation Godbout, Nathalie; Salahub, Dennis R.; Andzelm, Jan Canadian Journal of Chemistry, Vol. 70, Issue 2 https://doi.org/10.1139/v92-079	journal	February 1992
Computational Kinetic Discrimination of Ethylene Polymerization Mechanisms for the Phillips (Cr/SiO ₂ ) Catalyst Fong, Anthony; Yuan, Ye; Ivry, Sam L. ACS Catalysis, Vol. 5, Issue 6 https://doi.org/10.1021/acscatal.5b00016	journal	May 2015
Theoretical Investigations of Isolated Mo(VI) and Mo(IV) Centers of a Molybdena−Silica Catalyst for Olefin Metathesis Handzlik, Jarosław The Journal of Physical Chemistry C, Vol. 111, Issue 26 https://doi.org/10.1021/jp071568y	journal	July 2007
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Amorphous Silica Slab Models with Variable Surface Roughness and Silanol Density for Use in Simulations of Dynamics and Catalysis Wimalasiri, Pubudu N.; Nguyen, Nuong P.; Senanayake, Hasini S. The Journal of Physical Chemistry C, Vol. 125, Issue 42 https://doi.org/10.1021/acs.jpcc.1c06580	journal	October 2021
Molecular dynamics with coupling to an external bath Berendsen, H. J. C.; Postma, J. P. M.; van Gunsteren, W. F. The Journal of Chemical Physics, Vol. 81, Issue 8 https://doi.org/10.1063/1.448118	journal	October 1984
Computer Simulation of Liquids Allen, Michael P.; Tildesley, Dominic J. https://doi.org/10.1093/oso/9780198803195.001.0001	book	June 2017
Assessment of DFT Methods for Computing Activation Energies of Mo/W-Mediated Reactions Hu, Lianrui; Chen, Hui Journal of Chemical Theory and Computation, Vol. 11, Issue 10 https://doi.org/10.1021/acs.jctc.5b00373	journal	September 2015
Impact of Support Interactions for Single-Atom Molybdenum Catalysts on Amorphous Silica Ewing, Christopher S.; Bagusetty, Abhishek; Patriarca, Evan G. Industrial & Engineering Chemistry Research, Vol. 55, Issue 48 https://doi.org/10.1021/acs.iecr.6b03558	journal	November 2016
Accurate Prediction of Hydrocarbon Interactions with Zeolites Utilizing Improved Exchange-Correlation Functionals and QM/MM Methods: Benchmark Calculations of Adsorption Enthalpies and Application to Ethene Methylation by Methanol Gomes, Joseph; Zimmerman, Paul M.; Head-Gordon, Martin The Journal of Physical Chemistry C, Vol. 116, Issue 29 https://doi.org/10.1021/jp303321s	journal	July 2012
Introduction to Automatic Differentiation and MATLAB Object-Oriented Programming Neidinger, Richard D. SIAM Review, Vol. 52, Issue 3 https://doi.org/10.1137/080743627	journal	January 2010
Screening silica-confined single-atom catalysts for nonoxidative conversion of methane He, Shu-Yue; Li, Teng-Hao; Huang, Zheng-Qing The Journal of Chemical Physics, Vol. 154, Issue 17 https://doi.org/10.1063/5.0048962	journal	May 2021
Spontaneous Grafting of Nitrophenyl Groups on Amorphous Carbon Thin Films: A Structure–Reactivity Investigation Cullen, Ronan J.; Jayasundara, Dilushan R.; Soldi, Laura Chemistry of Materials, Vol. 24, Issue 6 https://doi.org/10.1021/cm2030262	journal	February 2012
Ethylene vinyl acetate based radiation grafted hydrophilic matrices: Process parameter standardization, grafting kinetics and characterization Chaudhari, C. V.; Mondal, R. K.; Dubey, K. A. Radiation Physics and Chemistry, Vol. 125 https://doi.org/10.1016/j.radphyschem.2016.04.017	journal	August 2016
Evidence that three-regime kinetics is inherent to formation of a polymer brush by a grafting-to approach Sha, Xue; Xu, Xiaohe; Sohlberg, Karl RSC Adv., Vol. 4, Issue 79 https://doi.org/10.1039/C4RA05663A	journal	January 2014
Kinetics of Low-Pressure Chemical Vapor Deposition of TiO[sub 2] from Titanium Tetraisopropoxide Siefering, K. L. Journal of The Electrochemical Society, Vol. 137, Issue 3 https://doi.org/10.1149/1.2086561	journal	January 1990
Chemical reactions at silica surfaces Morrow, B. A.; McFarlan, A. J. Journal of Non-Crystalline Solids, Vol. 120, Issue 1-3 https://doi.org/10.1016/0022-3093(90)90191-N	journal	April 1990
Advanced Surface Functionalization of Periodic Mesoporous Silica: Kinetic Control by Trisilazane Reagents Zapilko, Clemens; Widenmeyer, Markus; Nagl, Iris Journal of the American Chemical Society, Vol. 128, Issue 50 https://doi.org/10.1021/ja065444v	journal	December 2006
Silylation and surface properties of chemically grafted hydrophobic silica Capel-Sanchez, M. C.; Barrio, L.; Campos-Martin, J. M. Journal of Colloid and Interface Science, Vol. 277, Issue 1 https://doi.org/10.1016/j.jcis.2004.04.055	journal	September 2004

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