Mechanistic Insights into Copper(I) and Copper (II) Cation Exchange Reactions in CdSe Nanoplatelets

21 July 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

In this study, we investigated the synthesis of copper selenide nanoplatelets (NPLs) through a cation exchange reaction (CER) in 5 monolayers thick CdSe NPLs using Cu(I) and Cu(II) precursors. We discovered that the exposure of CdSe NPLs to Cu(I) precursor led to the transformation of NPLs into Cu2−xSe while maintaining their nanoplatelet morphology. The replacement of Cd(II) with Cu(I) prevailed over the formation of doped structures. In the case of Cu(II) precursor, we observed that Cu(II) was first reduced to Cu(I) before being intercalated into the host lattice, resulting in synthesis of Cu2−xSe, similar to CER with Cu(I) precursors but without preservation of the initial morphology of NPLs. Interestingly, the presence of oxygen was found to facilitate the cation exchange processes in CdSe NPLs, whereas a nitrogen atmosphere suppressed the CER. Despite the similar ionic sizes of Cu(I) and Cu(II), the substitution of Cd(II) with Cu(II) was found to be challenging, possibly due to the involvement of redox processes resulting in the significant deterioration of initial CdSe NPLs. We demonstrate that CER can achieve near-complete substitution of cadmium atoms with monovalent copper under room temperature. Understanding the processes involved in CERs is crucial for engineering more complex structures, such as high entropy nanoparticles involving cation exchange with different oxidation states and development of material synthesis using machine learning and artificial intelligence approaches.

Keywords

2D Nanoplatelets
Cation Exchange Reaction
Hard Acid-Soft Base
Cadmium Selenide
Copper Selenide

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