美国塔夫茨大学E. Charles H. Sykes团队报道了单原子合金丙烷脱氢催化剂的第一性原理设计。相关研究成果发表在2021年6月25日出版的《科学》。

多相催化剂的复杂性意味着预先设计新的催化材料是困难的，但是单原子合金催化剂的良好性能使得进行明确的理论建模和精确的表面科学实验成为可能。

该文报道了理论指导下丙烷脱氢制丙烯的铑铜（RhCu）单原子合金催化剂的发现。虽然一般认为Rh不适用于烷烃脱氢反应，但第一性原理计算表明Rh原子分散在Cu中，表现出低碳氢键活化势垒。表面科学实验证实了这些预测，这些结果共同为设计一种高活性、高选择性、耐结焦的RhCu纳米颗粒催化剂提供了依据，从而低温无氧化丙烷脱氢成为可能。

附：英文原文

Title: First-principles design of a single-atom–alloy propane dehydrogenation catalyst

Author: Ryan T. Hannagan, Georgios Giannakakis, Romain Réocreux, Julia Schumann, Jordan Finzel, Yicheng Wang, Angelos Michaelides, Prashant Deshlahra, Phillip Christopher, Maria Flytzani-Stephanopoulos, Michail Stamatakis, E. Charles H. Sykes

Issue&Volume: 2021/06/25

Abstract: The complexity of heterogeneous catalysts means that a priori design of new catalytic materials is difficult, but the well-defined nature of single-atom–alloy catalysts has made it feasible to perform unambiguous theoretical modeling and precise surface science experiments. Herein we report the theory-led discovery of a rhodium-copper (RhCu) single-atom–alloy catalyst for propane dehydrogenation to propene. Although Rh is not generally considered for alkane dehydrogenation, first-principles calculations revealed that Rh atoms disperse in Cu and exhibit low carbon-hydrogen bond activation barriers. Surface science experiments confirmed these predictions, and together these results informed the design of a highly active, selective, and coke-resistant RhCu nanoparticle catalyst that enables low-temperature nonoxidative propane dehydrogenation.

DOI: 10.1126/science.abg8389

Source: https://science.sciencemag.org/content/372/6549/1444