5 years ago

Minerals to Materials: Bulk Synthesis of Aqueous Aluminum Clusters and Their Use as Precursors for Metal Oxide Thin Films

Minerals to Materials: Bulk Synthesis of Aqueous Aluminum Clusters and Their Use as Precursors for Metal Oxide Thin Films
John F. Conley, Milton N. Jackson, Ryan H. Mansergh, Melanie A. Jenkins, Brantly L. Fulton, Darren W. Johnson, Juan C. Ramos, Vasily Gouliouk, Shannon W. Boettcher, Nichole M. Rogovoy, James E. Hutchison, Maceo T. Gutierrez-Higgins, Douglas A. Keszler, Cory K. Perkins
We describe a process to produce aqueous precursor solutions of the flat-Al13 hydroxo cluster (Al133-OH)62-OH)18(H2O)24(NO3)15) via stoichiometric dissolution of bulk Al(OH)3(s) in HNO3(aq). We highlight its facility by demonstrating high yields and large-scale synthesis. X-ray diffraction confirms formation of a single-phase product, and Raman spectra show characteristic O-Al-O vibrational modes, both techniques confirming the identity of the flat-Al13 cluster in the bulk. 27Al NMR spectroscopy and dynamic light scattering also confirm the presence of the cluster in aqueous solution. We show the as-prepared solution produces smooth and continuous thin films via spin-coating. In capacitors, the films exhibit low leakage currents (near 10 nA/cm2) and dielectric constants expected for amorphous Al2O3. Because the precursor preparation requires no postsynthesis purification, it is readily scalable to large volumes.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b02106

DOI: 10.1021/acs.chemmater.7b02106

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