Abstract
The detailed degree of mixing between framework Si and metal cations and the nature of oxygen that only links metal cations (metal-bridging oxygen) in archetypal metal oxide glasses have been among the unsolved problems in physical chemistry. Binary lead silicate (PbO-SiO2) glass is an ideal model system for exploring the extent of cation disorder and metal-bridging oxygen because of its peculiar glass-forming ability at high PbO concentration. Here we report the first high-resolution 17O solid-state NMR spectra for binary lead silicate glasses with varying composition (near that of orthosilicate, i.e., Pb/Si = 2), where peaks due to metal-bridging oxygen (Pb-O-Pb), as well as Pb-O-Si and Si-O-Si are clearly resolved. The spectra also reveals that the metal-bridging oxygen possesses a greater topological disorder due to structural complexity in Pb coordination environments. Together with a statistical thermodynamic model of oxygen speciation proposed to describe mixing behavior in oxide glasses with any o...
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