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High-entropy-inspired multi-principal single-atom materials
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DOI：10.1016/j.chempr.2026.103153.png)
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Abstract
En 中文
The design of single-atom materials (SAMs) is shifting from isolated active sites to multi-principal active spaces where coexisting metal atoms enable new catalytic functions, such as interatomic-promoted activation, site-to-site relay, and redox coupling. Such capabilities help overcome scaling relations in complex reactions. Within multi-principal SAMs (MPSAMs), including the more commonly known high-entropy SAMs, rigorous terminology and entropy-gradient experiments are essential to clarify entropic roles and establish predictable composition-activity relationships. Regarding synthesis strategies, the field is evolving from conventional pyrolysis to controlled entropy engineering, with approaches such as laser ablation, thermal shock, and cyanogel self-assembly providing access to metastable structures under extreme or mild conditions. These methods overcome thermodynamic miscibility limits or enable atomic-level control over size, morphology, defects, and element distribution. The expanded synthetic toolbox opens new possibilities for discovering MPSAMs with tailored structures and properties. In addition, understanding local order within globally disordered atomic arrangements is increasingly important. Although MPSAMs exhibit overall random distributions, emerging evidence points to short-range order, specific coordination preferences, or sub-nanometer metal-metal interactions that influence electronic structure and catalytic performance. Characterizing these local structures remains difficult because current techniques have inherent limitations in distinguishing true randomness from short-range ordering. Combining multiple characterization methods with theoretical modeling offers a practical path forward, though direct atomic-scale observation is still an ongoing pursuit.
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