Operando pair distribution function analysis of nanocrystalline functional materials: the case of $\mathrm{T}\mathrm{i}{\mathrm{O}}_2$-bronze nanocrystals in Li-ion battery electrodes

Structural modelling of $operando$ pair distribution function (PDF) data of functional materials can be highly complex. To aid the understanding of complex operando PDF data, we here demonstrate a toolbox for PDF analysis. The tools include the structureMining, similarityMapping, nmfMapping apps available through the online service ‘PDF in the cloud’ (PDFitc, www.pdfitc.org), as well as noise-filtering using principal component analysis (PCA). The tools are applied to both ex situ and operando PDF data for 3 nm $\mathrm{T}\mathrm{i}{\mathrm{O}}_2$-bronze nanocrystals, which function as the active electrode material in a Li-ion battery. The tools enable structural modelling of the ex situ and operando PDF data, revealing two pristine $\mathrm{T}\mathrm{i}{\mathrm{O}}_2$ phases (bronze and anatase) and two lithiated $\mathrm{L}{\mathrm{i}}_{\mathrm{x}}\mathrm{T}\mathrm{i}{\mathrm{O}}_2$ phases (lithiated versions of bronze and anatase), and the phase evolution during Galvanostatic cycling is characterized.