Publication date: 15th December 2025
High-entropy materials (HEMs) have emerged as a versatile platform for diverse applications, yet colloidal high-entropy chalcogenide nanocrystals (NCs) remain largely underexplored due to synthetic challenges owing to the reactivity disparities of multiple reactive species. Here, we report the first synthesis of monodisperse high-entropy Cu based chalcogenide NCs in the tetrahedrite phase, a flexible crystal structure that accommodates multiple cations with different valencies. A majority of HEMs rely on high temperature annealing to achieve a single, homogeneous phase stabilized by high configurational entropy. Employing a sequential, low-temperature cation-exchange strategy, we start with a Cu-Zn-Sb-S quaternary sulphide template and incorporate Ag⁺ and Bi³⁺ ions, preserving the crystal phase while enabling precise control over morphology. This bottom-up soft-chemistry approach circumvents the need for high-temperature enabling entropy-stabilized NCs with control over morphology. Remarkably, the synthesized NCs are fairly monodisperse, in contrast to conventional high-entropy systems that often suffer from particle aggregation and polydispersity. When evaluated as electrocatalysts, the high entropy tetrahedrite NCs demonstrate excellent hydrogen evolution reaction (HER) activity in acidic media, with low overpotentials and favorable Tafel slopes compared to their intermediate counterparts. This work introduces a new class of colloidal high-entropy chalcogenide NCs and establishes the first high-entropy tetrahedrite phase, paving the way for entropy-stabilized chalcogenide catalysts for energy conversion applications.
The financial support of Taighde Éireann – Research Ireland under Grant number 22/FFP-P/11591 and GOIPD/2024/600 are ackowledged.
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