期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-020-20712-0
关键词
-
资金
- National Science Foundation [DMR-1708617]
- Department of Energy (DOE)
- DOE Office of Science [DE-AC02-06CH11357]
This study investigates the mechanism of cation exchange in nanocrystals using in situ x-ray absorption spectroscopy, revealing evidence of interstitial intermediates and suggesting diffusion as the fundamental mechanism of cation exchange in this system.
In terms of producing new advances in sustainable nanomaterials, cation exchange (CE) of post-processed colloidal nanocrystals (NCs) has opened new avenues towards producing non-toxic energy materials via simple chemical techniques. The main processes governing CE can be explained by considering hard/soft acid/base theory, but the detailed mechanism of CE, however, has been debated and has been attributed to both diffusion and vacancy processes. In this work, we have performed in situ x-ray absorption spectroscopy to further understand the mechanism of the CE of copper in solution phase CdSe NCs. The x-ray data indicates clear isosbestic points, suggestive of cooperative behavior as previously observed via optical spectroscopy. Examination of the extended x-ray absorption fine structure data points to the observation of interstitial impurities during the initial stages of CE, suggesting the diffusion process is the fundamental mechanism of CE in this system. There currently exists some debate as to exact mechanism of cation exchange in semiconductor nanocrystals, a crucial question regarding the fundamental materials chemistry of these systems. Here, the authors report a detailed investigation of the mechanism of cation exchange in nanocrystals, which unambiguously shows evidence of interstitial intermediates during the exchange process.
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