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Halide Diffusion in MAPbX3: Limits to Topotaxy for Halide Exchange in Perovskites

卤化银 金属卤化物 化学 碘化物 卤素
作者
Aya Osherov,Yishay Feldman,Ifat Kaplan‐Ashiri,David Cahen,Gary Hodes
出处
期刊:Chemistry of Materials [American Chemical Society]
卷期号:32 (10): 4223-4231 被引量:16
标识
DOI:10.1021/acs.chemmater.0c00496
摘要

We study halide exchange in the prototypical halide perovskite, methylammonium lead trihalide, MAPbX3 (X = halide), to test and possibly experimentally use halide diffusion in these materials. We use macroscopic single crystals to study the fundamental exchange process(es) so as to minimize possible grain boundary and surface diffusion effects. Initially, halide exchange creates normal concentration gradients of the outgoing and incoming halides, on a scale of a few microns to a few hundred microns. The depth (from the surface) of the substituted volume depends on the halide pair and on which one is exchanged and which is exchanging. The concentration gradient of the incoming halides decreases from the crystal surface toward its inner core and vice versa for the out-going halides; the profiles roughly fit diffusion in a semi-infinite specimen. This concentration gradient changes slowly with time, with the crystal becoming more homogeneous with storage time. Using the Boltzmann–Matano method and diffusion profiles from electron-dispersive spectroscopy, we evaluate the halide diffusion coefficients; these are not constant and depend on the halide couple. Although these gradients cause a lattice parameter change and may cause a symmetry change, X-ray diffraction shows that if the exchanging halides are of similar size (e.g., Br– and Cl–, Br– and I–, but not Cl– and I–), the resulting material remains single crystalline, prima facie evidence for bulk halide diffusion. These findings are valid, irrespective of which is the exchanged halide. These results suggest that for the similar-sized halide pairs the solid-state chemical exchange is topotactic such that the resulting crystal orientation is determined by that of the initial crystal. I–Cl exchange leads to loss of single crystallinity, suggesting lack of miscibility, a finding that might bear on the difficulty in finding Cl in MAPbI3 samples grown from Cl-containing solutions.
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