Entropy-driven electronic reconfiguration in high-entropy sulfides enables rapid charge-transfer dynamics for next-generation wearable energy devices

초록

Sustainable energy research demands high-performance energy-storage systems to address the ongoing energy crisis. Among various electrode candidates, transition-metal sulfides have been extensively explored due to their high theoretical capacity and rich redox chemistry. However, conventional transition-metal sulfides face persistent challenges such as phase segregation, slow ion transport, and poor long-term stability, which hinder their practical application. To overcome these limitations, we propose a one-step pulsed laser irradiation in liquid strategy for synthesizing a phase-pure high-entropy sulfide (HES) based on the quinary (PbNiCoCuZn)S system. This HES exhibits exceptional tolerance to issues commonly associated with phase segregation, complex precursor chemistry, and hazardous reaction conditions. The rapid, nonequilibrium laser process enables the stabilization of a single-phase, entropy-driven quinary sulfide with homogeneous elemental distribution and electronic charge redistribution—features that are rarely achievable through conventional thermal routes. Beyond structural advantages, this approach directly produces nanoparticle suspensions with a configurational entropy (ΔSconf) of 1.58R, enabling the formulation of HES/PEDOT:PSS hybrid inks with well-defined compositional and electronic uniformity. Density functional theory calculations reveal entropy-driven bandgap narrowing in the high-entropy sulfide lattice, a reduced work function at the HES surface, and polymer-induced electronic delocalization across the HES/PEDOT:PSS interfacial region, together accounting for the accelerated charge-transfer kinetics in the HES/PEDOT:PSS electrode. The resulting hybrid electrode combines multielement redox activity with polymer-facilitated electronic delocalization and ionic transport, achieving a high areal capacitance of 728 mF cm−2. An asymmetric hybrid SC (AHSC) constructed from this material exhibits a wide operating voltage of 1.7 V and superior stability over 10000 cycles in a 6 M KOH aqueous electrolyte. A textile-wearable, flexible AHSC prototype, coupled with a flexible solar cell, maintains excellent mechanical integrity under bending, folding, and twisting conditions. Overall, this study establishes a generalizable manufacturing strategy for producing entropy-stabilized, phase-pure quinary sulfides, advancing the development of next-generation flexible energy-storage technologies. © 2026 Elsevier B.V.

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