Tailoring the Local Environment of Platinum in Single‐Atom Pt<sub>1</sub>/CeO<sub>2</sub> Catalysts for Robust Low‐Temperature CO Oxidation
Dong Jiang, Yonggang Yao, Tangyuan Li, Gang Wan, Xavier Isidro Pereira Hernández, Yubing Lu, Jinshu Tian, Konstantin Khivantsev, Mark Engelhard, Cheng‐Jun Sun, Carlos Garcia Vargas, Adam S. Hoffman, Simon R. Bare, Abhaya K. Datye, Liangbing Hu, Yong Wang
Abstract
Abstract A single‐atom Pt 1 /CeO 2 catalyst formed by atom trapping (AT, 800 °C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over‐stabilization of Pt 2+ in a highly symmetric square‐planar Pt 1 O 4 coordination environment. Reductive activation to form Pt nanoparticles (NPs) results in enhanced activity; however, the NPs are easily oxidized, leading to drastic activity loss. Herein we show that tailoring the local environment of isolated Pt 2+ by thermal‐shock (TS) synthesis leads to a highly active and thermally stable Pt 1 /CeO 2 catalyst. Ultrafast shockwaves (>1200 °C) in an inert atmosphere induced surface reconstruction of CeO 2 to generate Pt single atoms in an asymmetric Pt 1 O 4 configuration. Owing to this unique coordination, Pt 1 δ+ in a partially reduced state dynamically evolves during CO oxidation, resulting in exceptional low‐temperature performance. CO oxidation reactivity on the Pt 1 /CeO 2 _TS catalyst was retained under oxidizing conditions.