Understanding the Formation Mechanisms of Silicon Particles from the Thermal Disproportionation of Hydrogen Silsesquioxane.

Autor: Cibaka-Ndaya C; Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France., O'Connor K; Department of Chemistry, University of Alberta, Edmonton, Alberta T6G 2G2, Canada., Idowu EO; Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France., Parker MA; Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France., Lebraud E; Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France., Lacomme S; Univ. Bordeaux, CNRS, INSERM, Bordeaux Imaging Center, UAR 3420, F-33600 Pessac, France., Montero D; Sorbonne Université, CNRS, Fédération de Chimie et Matériaux de Paris-Centre, FR 2482, 75252 Paris, France., Camacho PS; Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France., Veinot JG; Department of Chemistry, University of Alberta, Edmonton, Alberta T6G 2G2, Canada., Roiban IL; Univ. Lyon, INSA Lyon, Université Claude Bernard Lyon 1, CNRS, MATEIS, UMR5510, 69621 Villeurbanne, France., Drisko GL; Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France.
Jazyk: angličtina
Zdroj: Chemistry of materials : a publication of the American Chemical Society [Chem Mater] 2023 Oct 11; Vol. 35 (20), pp. 8551-8560. Date of Electronic Publication: 2023 Oct 11 (Print Publication: 2023).
DOI: 10.1021/acs.chemmater.3c01448
Abstrakt: Crystalline silicon particles sustaining Mie resonances are readily obtained from the thermal processing of hydrogen silsesquioxane (HSQ). Here, the mechanisms involved in silicon particle formation and growth from HSQ are investigated through real-time in situ analysis using an environmental transmission electron microscope and X-ray diffractometer. The nucleation of Si nanodomains is observed starting around 1000 °C. For the first time, a highly mobile intermediate phase is experimentally observed, thus demonstrating a previously unknown growth mechanism. At least two growth processes occur simultaneously: the coalescence of small particles into larger particles and growth mode by particle displacement through the matrix toward the HSQ grain surface. Postsynthetic characterization by scanning electron microscopy further supports the latter growth mechanism. The gaseous environment employed during synthesis impacts particle formation and growth under both in situ and ex situ conditions, impacting the particle yield and structural homogeneity. Understanding the formation mechanisms of particles provides promising pathways for reducing the energy cost of this synthetic route.
Competing Interests: The authors declare no competing financial interest.
(© 2023 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE