Phosphine-Free Synthesis of Metal Chalcogenide Quantum Dots by Directly Dissolving Chalcogen Dioxides in Alkylthiol as the Precursor

ACS Appl Mater Interfaces. 2017 Mar 22;9(11):9840-9848. doi: 10.1021/acsami.6b16407. Epub 2017 Mar 9.

Abstract

Semiconductor quantum dots (QDs) are competitive emitting materials in developing new-generation light-emitting diodes (LEDs) with high color rendering and broad color gamut. However, the use of highly toxic alkylphosphines cannot be fully avoided in the synthesis of metal selenide and telluride QDs because they are requisite reducing agents and solvents for preparing chalcogen precursors. In this work, we demonstrate the phosphine-free preparation of selenium (Se) and tellurium (Te) precursors by directly dissolving chalcogen dioxides in the alkylthiol under the mild condition. The chalcogen dioxides are reduced to elemental chalcogen clusters, while the alkylthiol is oxidized to disulfides. The chalcogen clusters further combine with the disulfides, generating dispersible chalcogen precursors. The resulting chalcogen precursors are suitable for synthesizing various metal chalcogenide QDs, including CdSe, CdTe, Cu2Te, Ag2Te, PbTe, HgTe, and so forth. In addition, the precursors are of high reactivity, which permits a shorter QD synthesis process at lower temperature. Owing to the high quantum yield (QYs) and easy tunability of the photoluminescence (PL), the as-synthesized QDs are further employed as down-conversion materials to fabricate monochrome and white LEDs.

Keywords: chalcogen precursors; light-emitting diodes; metal selenide/telluride nanocrystals; phosphine-free synthesis; quantum dots.