Distinct Role of Surface Hydroxyls in Single-Atom Pt1/CeO2 Catalyst for Room-Temperature Formaldehyde Oxidation: Acid-Base Versus Redox

Lina Zhang; Qianqian Bao; Bangjie Zhang; Yuanbao Zhang; Shaolong Wan; Shuai Wang; Jingdong Lin; Haifeng Xiong; Donghai Mei; Yong Wang

doi:10.1021/jacsau.2c00215

Distinct Role of Surface Hydroxyls in Single-Atom Pt₁/CeO₂ Catalyst for Room-Temperature Formaldehyde Oxidation: Acid-Base Versus Redox

JACS Au. 2022 Jun 10;2(7):1651-1660. doi: 10.1021/jacsau.2c00215. eCollection 2022 Jul 25.

Authors

Lina Zhang^{1

2}, Qianqian Bao³, Bangjie Zhang^{1

2}, Yuanbao Zhang^{1

2}, Shaolong Wan^{1

2}, Shuai Wang^{1

2}, Jingdong Lin^{1

2}, Haifeng Xiong^{1

2}, Donghai Mei³, Yong Wang⁴

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
² National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
³ State Key Laboratory of Separation Membranes and Membrane Processes, School of Chemical Engineering and Technology, Tiangong University, Tianjin 300387, China.
⁴ Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, Washington 99164, United States.

Abstract

The development of highly efficient catalysts for room-temperature formaldehyde (HCHO) oxidation is of great interest for indoor air purification. In this work, it was found that the single-atom Pt₁/CeO₂ catalyst exhibits a remarkable activity with complete removal of HCHO even at 288 K. Combining density functional theory calculations and in situ DRIFTS experiments, it was revealed that the active O_latticeH site generated on CeO₂ in the vicinity of Pt²⁺ via steam treatment plays a key role in the oxidation of HCHO to formate and its further oxidation to CO₂. Such involvement of hydroxyls is fundamentally different from that of cofeeding water which dissociates on metal oxide and catalyzes the acid-base-related chemistry. This study provides an important implication for the design and synthesis of supported Pt catalysts with atom efficiency for a very important practical application-room-temperature HCHO oxidation.