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DOE OSTI · 1976956

Vapor-phase self-assembly for generating thermally stable single-atom catalysts

Li, Hengyu·Wan, Qiang·Du, CongCong·Liu, QiuNan·Qi, Jiamin·Ding, Xingyu·Wang, Shuai·Wan, Shaolong·Lin, Jingdong·Tian, Chen·Li, Lina·Peng, Tao·Zhao, Wei·Zhang, Kelvin H. L.·Huang, Jianyu·Zhang, Xiaoben·Gu, Qingqing·Yang, Bing·Guo, Hua·Lin, Sen·Datye, Abhaya K.·Wang, Yong·Xiong, Haifeng
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Abstract

Preparation of thermally stable metal single-atom catalysts (SACs) is a challenge in heterogeneous catalysis, especially on conventional supports that provide a weak metal-support interaction. In this work, we report that a modified support MgAl 2 O 4 can stabilize Pt single atoms by a mechanism of vapor-phase self-assembly in a high-temperature treatment (800°C, air). The experimental results on the formation mechanism and the structure are validated by DFT and ab initio molecular dynamics simulations. We infer that stable triangular K 3 O 3 structures help stabilize Pt single atoms at high temperatures in oxidizing conditions, exhibiting excellent reactivity for methane oxidation. The obtained Pt/K/MgAl 2 O 4 SAC presents excellent stability in methane oxidation after steam treatment at elevated temperatures, whereas the Pt/MgAl 2 O 4 nanocatalyst suffers from rapid deactivation due to Pt nanoparticle growth. Now this work paves the way for preparing thermally stable and highly active SACs using conventional high-surface-area supports, despite the weak metal-support interaction.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYPt/MgAl2O4 single-atom catalystSACsatom trappingmobile speciessurface functionalizationthermal stabilityvapor-phase self-assemblyweak metal-support interaction

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Li, Hengyu, Wan, Qiang, Du, CongCong, Liu, QiuNan, Qi, Jiamin, Ding, Xingyu, Wang, Shuai, Wan, Shaolong, Lin, Jingdong, Tian, Chen, Li, Lina, Peng, Tao, Zhao, Wei, Zhang, Kelvin H. L., Huang, Jianyu, Zhang, Xiaoben, Gu, Qingqing, Yang, Bing, Guo, Hua, Lin, Sen, Datye, Abhaya K., Wang, Yong, Xiong, Haifeng. 2021-11-29. Vapor-phase self-assembly for generating thermally stable single-atom catalysts. https://doi.org/10.1016/j.chempr.2021.11.002

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