Template-Induced Structuring and Tunable Polymorphism of Three-Dimensionally Ordered Mesoporous (3DOm) Metal Oxides

Gregory, Daniel G.; Guo, Qianying; Lu, Li; Kiely, Christopher J.; Snyder, Mark A.

doi:10.1021/acs.langmuir.7b01112

Title: Template-Induced Structuring and Tunable Polymorphism of Three-Dimensionally Ordered Mesoporous (3DOm) Metal Oxides

Journal Article · Mon Jun 12 00:00:00 EDT 2017 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.7b01112· OSTI ID:1469843

Gregory, Daniel G. ^[1]; Guo, Qianying ^[2];

^[3]; Kiely, Christopher J. ^[4];

^[2]

Lehigh Univ., Bethlehem, PA (United States). Dept. of Chemical and Biomolecular Engineering
Lehigh Univ., Bethlehem, PA (United States). Dept. of Chemical and Biomolecular Engineering
Department of Chemical and Biomolecular Engineering and ‡Department of Materials Science and Engineering, Lehigh University, Bethlehem, Pennsylvania 18015, United States
Lehigh Univ., Bethlehem, PA (United States). Dept. of Chemical and Biomolecular Engineering, and Dept. of Materials Science and Engineering

Convectively assembled colloidal crystal templates, comprised of size-tunable (ca. 15-50 nm) silica (SiO₂) nanoparticles, enable versatile sacrificial templating of three-dimensionally ordered mesoporous (3DOm) metal oxides (MO_x) at both mesoscopic and microscopic size-scales. Specifically, we show for titania (TiO₂) and zirconia (ZrO₂) how this approach not only enables the engineering of the mesopore size, pore volume, and surface area but can also be leveraged to tune crystallite polymorphism of the resulting 3DOm metal oxides. Template-mediated volumetric (i.e., interstitial) effects and interfacial factors are shown to preserve the metastable crystalline polymorphs of each corresponding 3DOm oxide (i.e., anatase TiO₂ (A-TiO₂) and tetragonal ZrO₂ (t-ZrO₂)) during high-temperature calcination. Mechanistic investigations suggest that this polymorph stabilization is derived from the combined effects of the templatereplica (MO_x/SiO₂) interface and simultaneous interstitial confinement that limits the degree of coarsening during high temperature calcination of the template-replica composite. The result is the identification of a facile yet versatile templating strategy for realizing 3DOm oxides with (i) surface areas that are more than an order of magnitude larger than those untemplated control samples, (ii) pore diameters and volumes that can be tuned across a continuum of size-scales, and (iii) selectable polymorphism.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001004

OSTI ID:: 1469843

Journal Information:: Langmuir, Vol. 33, Issue 26; Related Information: CCEI partners with the University of Delaware (lead); Brookhaven National Laboratory; California Institute of Technology; Columbia University; University of Delaware; Lehigh University; University of Massachusetts, Amherst; Massachusetts Institute of Technology; University of Minnesota; Pacific Northwest National Laboratory; University of Pennsylvania; Princeton University; Rutgers University; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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Title: Template-Induced Structuring and Tunable Polymorphism of Three-Dimensionally Ordered Mesoporous (3DOm) Metal Oxides

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