High-entropy-inspired multi-principal single-atom materials

Emerging multi-principal single-atom materials (MPSAMs), including commonly known high-entropy single-atom materials, extend the design principles of high-entropy alloys into atomically dispersed frameworks. This perspective examines the developmental pathway of MPSAMs and describes how combining insights from high-entropy and related fields with the atomic precision of single-atom materials leads to unconventional reactivity patterns. We suggest that a range of observable features, from basic composition to specific structural and functional characteristics, can be used to inform entropy-inspired design of MPSAMs for nonlinear synergistic performance. Following the concept of chemical short-range order in alloy physics, a promising direction is to modulate the metal atom arrangement from completely random to partially correlated states, enabling tailored local ordering in MPSAMs. The advancement requires expanding synthetic protocols and developing multidisciplinary platforms that integrate complementary characterization, theoretical cross-validation, and automated workflows to achieve predictive catalyst screening and rational design. © 2026 Elsevier Inc. All rights are reserved, including those for text and data mining, AI training, and similar technologies.