Wang Tao, Li Guomin, Cui Xinjiang, Abild-Pedersen Frank
SUNCAT Center for Interface Science and Catalysis, Stanford Linear Accelerator Center, Menlo Park, CA 94025.
Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024, Zhejiang Province, China.
Proc Natl Acad Sci U S A. 2021 Mar 16;118(11). doi: 10.1073/pnas.2024666118.
Selective ethane dehydrogenation (EDH) is an attractive on-purpose strategy for industrial ethylene production. Design of an effective, stable, and earth-abundant catalyst to replace noble metal Pt is the main obstacle for its large-scale application. Herein, we report an experimentally validated theoretical framework to discover promising catalysts for EDH, which combines descriptor-based microkinetic modeling, high-throughput computations, machine-learning concepts, and experiments. Our approach efficiently evaluates 1,998 bimetallic alloys by using accurately calculated C and CH adsorption energies and identifies a small number of new promising noble-metal-free catalysts for selective EDH. A NiMo alloy predicted to be promising is successfully synthesized, and experimentally proven to outperform Pt in selective ethylene production from EDH, representing an important contribution to the improvement of light alkane dehydrogenation to olefins. These results will provide essential additions in the discovery and application of earth-abundant materials in catalysis.
选择性乙烷脱氢（EDH）是一种颇具吸引力的用于工业乙烯生产的定向策略。设计一种有效、稳定且储量丰富的催化剂来替代贵金属铂是其大规模应用的主要障碍。在此，我们报告了一个经过实验验证的理论框架，用于发现有前景的EDH催化剂，该框架结合了基于描述符的微观动力学建模、高通量计算、机器学习概念和实验。我们的方法通过使用精确计算的C和CH吸附能有效评估了1998种双金属合金，并识别出少量用于选择性EDH的新型有前景的无贵金属催化剂。一种预测有前景的NiMo合金被成功合成，并通过实验证明在EDH选择性生产乙烯方面优于铂，这对将轻质烷烃脱氢制烯烃的改进具有重要贡献。这些结果将为储量丰富的材料在催化领域的发现和应用提供重要补充。
