Overcoming Limitations in the Strong Interaction between Pt and Irreducible SiO2 Enables Efficient and Selective Hydrogenation of Anthracene

Xiao Chen; Xing-Bao Wang; Shuhua Han; Dong Wang; Chuang Li; Weixiang Guan; Wen-Ying Li; Changhai Liang

doi:10.1021/acsami.1c16965

Overcoming Limitations in the Strong Interaction between Pt and Irreducible SiO₂ Enables Efficient and Selective Hydrogenation of Anthracene

ACS Appl Mater Interfaces. 2022 Jan 12;14(1):590-602. doi: 10.1021/acsami.1c16965. Epub 2021 Dec 14.

Authors

Xiao Chen¹, Xing-Bao Wang², Shuhua Han¹, Dong Wang¹, Chuang Li¹, Weixiang Guan¹, Wen-Ying Li³, Changhai Liang¹

Affiliations

¹ State Key Laboratory of Fine Chemicals, Laboratory of Advanced Materials and Catalytic Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
² Training Base of State Key Laboratory of Coal Science and Technology Jointly Constructed by Shanxi Province and Ministry of Science and Technology, Taiyuan University of Technology, Taiyuan 030024, China.
³ State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China.

PMID: 34905332
DOI: 10.1021/acsami.1c16965

Abstract

Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal-support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO₂ supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt-SiO₂ interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO₂ has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the Pt₂Si/SiO₂ catalyst with an initial catalytic activity of 2.49 μmol/(m²/g)/h as well as TOF of 0.95 s^-1 preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (sym-OHA) by subsequent hydrogenation. In addition, the Pt₂Si/SiO₂ catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic Pt₂Si nanoparticles are anchored firmly onto the surface of the SiO₂ support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal-SiO₂ interface and tune the surface chemical properties in diverse application conditions.

Keywords: anthracene; electrostatic adsorption; selective hydrogenation; silicide; strong metal−support interactions.