Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts

YG Yao and ZY Liu and PF Xie and ZN Huang and TY Li and D Morris and Z Finfrock and JH Zhou and ML Jiao and JL Gao and YM Mao and JW Miao and P Zhang and R Shahbazian-Yassar and C Wang and GF Wang and LB Hu, SCIENCE ADVANCES, 6, eaaz0510 (2020).

DOI: 10.1126/sciadv.aaz0510

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.

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