Construction of Active Site in a Sintered Copper-Ceria Nanorod Catalyst

Wen-Zhu Yu; Wei-Wei Wang; Shan-Qing Li; Xin-Pu Fu; Xu Wang; Ke Wu; Rui Si; Chao Ma; Chun-Jiang Jia; Chun-Hua Yan

doi:10.1021/jacs.9b05419

Construction of Active Site in a Sintered Copper-Ceria Nanorod Catalyst

J Am Chem Soc. 2019 Nov 6;141(44):17548-17557. doi: 10.1021/jacs.9b05419. Epub 2019 Oct 25.

Authors

Wen-Zhu Yu¹, Wei-Wei Wang¹, Shan-Qing Li², Xin-Pu Fu¹, Xu Wang³, Ke Wu^{4

5}, Rui Si³, Chao Ma⁶, Chun-Jiang Jia¹, Chun-Hua Yan^{4

5}

Affiliations

¹ Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering , Shandong University , Jinan 250100 , China.
² Department of Chemistry and Materials Engineering , Chizhou University , Chizhou 247000 , China.
³ Shanghai Synchrotron Radiation Facility , Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201204 , China.
⁴ Beijing National Laboratory for Molecular Sciences, State Key Lab of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Lab in Rare Earth Materials and Bioinorganic Chemistry , Peking University , Beijing 100871 , China.
⁵ College of Chemistry and Chemical Engineering , Lanzhou University , Lanzhou 730000 , China.
⁶ College of Materials Science and Engineering , Hunan University , Changsha 410082 , China.

PMID: 31607122
DOI: 10.1021/jacs.9b05419

Abstract

The construction of stable active site in nanocatalysts is of great importance but is a challenge in heterogeneous catalysis. Unexpectedly, coordination-unsaturated and atomically dispersed copper species were constructed and stabilized in a sintered copper-ceria catalyst through air-calcination at 800 °C. This sintered copper-ceria catalyst showed a very high activity for CO oxidation with a CO consumption rate of 6100 μmol_CO·g_Cu^-1·s^-1 at 120 °C, which was at least 20 times that of other reported copper catalysts. Additionally, the excellent long-term stability was unbroken under the harsh cycled reaction conditions. Based on a comprehensive structural characterization and mechanistic study, the copper atoms with unsaturated coordination in the form of Cu₁O₃ were identified to be the sole active site, at which both CO and O₂ molecules were activated, thus inducing remarkable CO oxidation activity with a very low copper loading (1 wt %).

Publication types

Research Support, Non-U.S. Gov't