Rational Design of Transition Metal Co‐Doped Ceria Catalysts for Low‐Temperature CO Oxidation

Abstract We present a highly active CeO 2 ‐based catalyst for oxidizing CO in automobile exhaust. This catalyst was systemically designed by co‐doping with transition metals (TMs). First, we used density functional theory (DFT) calculations to screen Mn and 13 dopant TMs (periods 4∼6 in groups VIII∼XI) and their 91 binary combinations for co‐doping. As a result, Cu and (Cu, Ag) were found to be the best candidates among the single and binary dopants, respectively. Next, we synthesized CeO 2 nanoparticles doped with Cu or (Cu, Ag), then experimentally confirmed that the predicted (Cu, Ag) co‐doped CeO 2 showed higher activity than pure CeO 2 and other TM‐doped CeO 2 . This was attributed to the easy formation of oxygen vacancies in the lattice of CeO 2 . Our study demonstrates that the use of a rational design of CeO 2 ‐based catalyst through theoretical calculations and experimental validation can effectively improve the low‐temperature catalytic activity of CO oxidation.