Decoding the entropy-stabilized matrix of high-entropy layered double hydroxides: Harnessing strain dynamics for...

The current understanding of the mechanism of high-entropy layered double hydroxide (LDH) on enhancing the efficiency of activating peroxymonosulfate (PMS) remains limited. This work reveals that a strong strain effect, driven by high entropy, modulates the structure of FeCoNiCuZn-LDH (HE-LDH) as evidenced by geometric phase analysis (GPA) and density functional theory (DFT) calculations. Compared to FeCoNiZn-LDH and FeCoNi-LDH with weaker strain effects, the high entropy-driven strain effect in HE-LDH shortens metal-oxygen-hydrogen (MOH) bond lengths, allows system to be in a constant steady state during catalysis, reduces the leaching of active M-OH sites, and enhances the adsorption capacity of these sites and the excess strain strength of the interfacial stretches the I_O-O of the PMS, facilitates reactive oxygen species (·OH, SO₄·^-, ¹O₂ and O₂·^-) generation, and thereby improving the efficiency of PMS in degrading tetracycline (TC). Consequently, HE-LDH demonstrated a 90% TC degradation within 3 min, maintained over 92% TC removal across a wide pH range (3-11), and achieved over 90% degradation performance after 6 cycles. This study reports the first use of high-entropy LDH material as a non-homogeneous catalyst and provides insights into the extremely different catalytic behaviors of high entropy mechanisms for the activation of PMS.