Computational Analysis of the Energetic Stability of High-Entropy Structures of a Prototypical Lanthanide-Based Metal–Organic Framework

Abstract

High-entropy materials are characterized by their complex compositions, typically comprising five or more elements in near-equiatomic proportions. Applying this concept to metal ions in metal–organic frameworks (MOFs) has paved the way for exploring a new class of high-entropy MOFs. While the compositional strategy of high-entropy materials leverages configurational entropy to aid thermodynamic stability, it also poses significant analytical challenges due to the vast compositional landscape and diverse phases that these materials can adopt. We present a computational study of several complexities associated with selecting potential high-entropy versions of a prototype lanthanide-based MOF. We compute the energetics of metal mixing of these heterometallic MOFs using density functional theory (DFT) and machine learning interatomic potential (MLIP) methods. The use of MLIP methods allows a systematic exploration of the convex hull of thermodynamically stable MOF structures containing up to 5 distinct metals.