Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts
Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts
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DOI：
10.1126/sciadv.aaz0510
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发表时间：
2020-03-01
期刊：
影响因子：
13.6
通讯作者：
Hu, Liangbing
中科院分区：
文献类型：
--
作者：
Yao, Yonggang;Liu, Zhenyu;Hu, Liangbing
多元素合金纳米颗粒（MEA-NP）在几乎无限的组成空间中为催化剂的发现带来了巨大的希望。然而，这些本质上复杂的结构的合理且可控的合成仍然是一个挑战。在这里，我们报告了高效耐用的催化剂 MEA-NP 的计算辅助、熵驱动设计和合成。计算策略包括预先筛选数百万种成分、通过密度泛函理论计算预测合金形成，以及通过混合蒙特卡罗和分子动力学方法检查结构稳定性。选定的组合物可以在高温（例如1500 K，0.5 s）下高效快速地合成，并具有优异的热稳定性。我们将这些 MEA-NPs 用于催化 NH3 分解，并观察到由于多元素混合的协同效应、它们的小尺寸和合金相而表现出出色的性能。我们预计 MEA-NP 的计算辅助合理设计和快速合成将广泛适用于各种催化反应，并将加速材料发现。
Multi-elemental alloy nanoparticles (MEA-NPs) hold great promise for catalyst discovery in a virtually unlimited compositional space. However, rational and controllable synthesize of these intrinsically complex structures remains a challenge. Here, we report the computationally aided, entropy-driven design and synthesis of highly efficient and durable catalyst MEA-NPs. The computational strategy includes pre-screening of millions of compositions, prediction of alloy formation by density functional theory calculations, and examination of structural stability by a hybrid Monte Carlo and molecular dynamics method. Selected compositions can be efficiently and rapidly synthesized at high temperature (e.g., 1500 K, 0.5 s) with excellent thermal stability. We applied these MEA-NPs for catalytic NH3 decomposition and observed outstanding performance due to the synergistic effect of multi-elemental mixing, their small size, and the alloy phase. We anticipate that the computationally aided rational design and rapid synthesis of MEA-NPs are broadly applicable for various catalytic reactions and will accelerate material discovery.