Controlling Activity of Heterogeneous Cu Single‐Atom Catalysts by Fine‐Tuning the Redox Properties of CeO2‐TiO2 Supports

Author:

Abdel‐Mageed Ali M.12ORCID,Cisneros Sebastian1,Mosrati Jawaher1,Atia Hanan1,Vuong Thanh Huyen1,Rockstroh Nils1,Wohlrab Sebastian1,Brückner Angelika13,Rabeah Jabor1

Affiliation:

1. Leibniz-Institut für Katalyse Albert-Einstein-Str. 29 A 18059 Rostock Germany

2. Department of Chemistry Faculty of Science Cairo University 1 Gamaa Street 12613 Giza Egypt

3. Interdisciplinary faculty Life, Light and Matter University of Rostock Albert-Einstein-Str. 21 18059 Rostock Germany

Abstract

AbstractUnderstanding and enhancing the activity of heterogeneous single‐atom catalysts (SACs) are indispensable aspects to use them in industrial applications. Among these, low‐temperature CO oxidation is considered as a model reaction for testing a wide‐range of oxidation catalysts, and as an essential process for the exhaust aftertreatment in modern combustion engines. This study demonstrates that the activity of heterogeneous Cu/CeO2−TiO2 SAC catalysts can be fine‐tuned by controlling the Ce/Ti ratio in CeO2−TiO2 supports, with the highest catalytic activity achieved for a Ce/Ti molar ratio of 0.18. Based on DRIFT, EEL, and EPR spectroscopies, together with high‐resolution electron microscopy and H2‐TPR measurements, it is inferred that the optimized Ce/Ti ratio correlates with i) highest dispersion of separate CeO2 particles on TiO2 surface, ii) more facile reduction of Ce4+ to Ce3+, and iii) enhanced formation of −Cu2+−O−Ce4+−⇆−Cu+−□−Ce3+− redox shuttles, which play a dual role for CO adsorption and O2‐activation. These results extend the understanding of heterogeneous metal single‐atom catalysts and constitute a robust approach for the rational control of their catalytic performance in technically relevant applications.

Publisher

Wiley

Subject

Inorganic Chemistry,Organic Chemistry,Physical and Theoretical Chemistry,Catalysis

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