Building Materials from Colloidal Nanocrystal Assemblies: Molecular Control of Solid/Solid Interfaces in Nanostructured Tetragonal ZrO2

Shaw, Santosh; Silva, Tiago F.; Bobbitt, Jonathan M.; Naab, Fabian; Rodrigues, Cleber L.; Yuan, Bin; Chang, Julia J.; Tian, Xinchun; Smith, Emily A.; Cademartiri, Ludovico

doi:10.1021/acs.chemmater.7b02769

Title: Building Materials from Colloidal Nanocrystal Assemblies: Molecular Control of Solid/Solid Interfaces in Nanostructured Tetragonal ZrO₂

Journal Article · Mon Aug 28 00:00:00 EDT 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b02769· OSTI ID:1399482

Shaw, Santosh ^[1]; Silva, Tiago F. ^[2]; Bobbitt, Jonathan M. ^[3]; Naab, Fabian ^[4]; Rodrigues, Cleber L. ^[2]; Yuan, Bin ^[5]; Chang, Julia J. ^[1]; Tian, Xinchun ^[1];

^[3];

^[6]

Iowa State Univ., Ames, IA (United States). Dept. of Materials Science and Engineering
Univ. of Sao Paulo (Brazil). Inst. of Physics
Iowa State Univ., Ames, IA (United States). Dept. of Chemistry; Ames Lab., Ames, IA (United States)
Univ. of Michigan, Ann Arbor, MI (United States). Michigan Ion Beam Lab.
Iowa State Univ., Ames, IA (United States). Dept. of Chemical and Biological Engineering
Iowa State Univ., Ames, IA (United States). Dept. of Materials Science and Engineering. Dept. of Chemical and Biological Engineering; Ames Lab., Ames, IA (United States)

We describe in this paper a bottom-up approach to control the composition of solid/solid interfaces in nanostructured materials, and we test its effectiveness on tetragonal ZrO₂, an inorganic phase of great technological significance. Colloidal nanocrystals capped with trioctylphosphine oxide (TOPO) or oleic acid (OA) are deposited, and the organic fraction of the ligands is selectively etched with O₂ plasma. The interfaces in the resulting all-inorganic colloidal nanocrystal assemblies are either nearly bare (for OA-capped nanocrystals) or terminated with phosphate groups (for TOPO-capped nanocrystals) resulting from the reaction of phosphine oxide groups with plasma species. The chemical modification of the interfaces has extensive effects on the thermodynamics and kinetics of the material. Different growth kinetics indicate different rate limiting processes of growth (surface diffusion for the phosphate-terminated surfaces and dissolution for the “bare” surfaces). Phosphate termination led to a higher activation energy of growth, and a 3-fold reduction in interfacial energy, and facilitated significantly the conversion of the tetragonal phase into the monoclinic phase. Finally, films devoid of residual ligands persisted in the tetragonal phase at temperatures as high as 900 °C for 24 h.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Semiconductor Research Corporation (United States)

Grant/Contract Number:: AC02-07CH11358; 2015-IN-2582

OSTI ID:: 1399482

Report Number(s):: IS-J9338

Journal Information:: Chemistry of Materials, Vol. 29, Issue 18; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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