High-entropy alloy nanoparticles (HEA-NPs) show exceptional properties and great potential as a new generation of functional materials, yet a universal and facile synthetic strategy in air toward nonoxidized and precisely controlled composition remains a huge challenge. Here we provide a laser scribing method to prepare single-phase solid solution HEA-NPs libraries in air with tunable composition at the atomic level, taking advantage of the laser-induced metastable thermodynamics and substrate-assisted confinement effect. The three-dimensional porous graphene substrate functions as a microreactor during the fast heating/cooling process, which is conductive to the generation of the pure alloy phase by effectively blocking the binding of oxygen and metals, but is also beneficial for realizing accurate composition control via microstructure confinement-endowed favorable vapor pressure. Furthermore, by combining an active learning approach based on an adaptive design strategy, we discover an optimal composition of quinary HEA-NP catalysts with an ultralow overpotential for Li-CO₂ batteries. This method provides a simple, fast, and universal in-air route toward the controllable synthesis of HEA-NPs, potentially integrated with machine learning to accelerate the research on HEAs.

中文翻译：

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激光精密合成无氧化高熵合金纳米粒子库


高熵合金纳米粒子（HEA-NP）作为新一代功能材料显示出优异的性能和巨大潜力，但在空气中实现非氧化和精确控制成分的通用且简便的合成策略仍然是一个巨大的挑战。在这里，我们提供了一种激光划片方法，利用激光诱导的亚稳态热力学和基底辅助限制效应，在空气中制备具有原子水平可调成分的单相固溶体 HEA-NPs 库。三维多孔石墨烯基底在快速加热/冷却过程中起到微反应器的作用，有效阻止氧与金属的结合，有利于纯合金相的生成，同时也有利于通过微观结构限制赋予了有利的蒸气压。此外，通过结合基于自适应设计策略的主动学习方法，我们发现了具有超低过电势的五元 HEA-NP 催化剂的最佳组合，适用于 Li-CO ₂ 电池。该方法为 HEA-NP 的可控合成提供了一种简单、快速且通用的空中途径，有可能与机器学习相结合，以加速 HEA 的研究。