Modulating the Electronic Metal-Support Interactions in Single-Atom Pt1 -CuO Catalyst for Boosting Acetone Oxidation

Zeyu Jiang; Mingjiao Tian; Meizan Jing; Shouning Chai; Yanfei Jian; Changwei Chen; Mark Douthwaite; Lirong Zheng; Mudi Ma; Weiyu Song; Jian Liu; Jiaguo Yu; Chi He

doi:10.1002/anie.202200763

Modulating the Electronic Metal-Support Interactions in Single-Atom Pt₁ -CuO Catalyst for Boosting Acetone Oxidation

Angew Chem Int Ed Engl. 2022 Jul 11;61(28):e202200763. doi: 10.1002/anie.202200763. Epub 2022 May 13.

Authors

Zeyu Jiang^{1

2}, Mingjiao Tian^{1

3}, Meizan Jing⁴, Shouning Chai¹, Yanfei Jian¹, Changwei Chen¹, Mark Douthwaite⁵, Lirong Zheng⁶, Mudi Ma¹, Weiyu Song⁴, Jian Liu⁴, Jiaguo Yu³, Chi He^{1

7}

Affiliations

¹ State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, Shaanxi, P. R. China.
² Department of Chemistry, National University of Singapore, Singapore, 117543, Singapore.
³ Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan, 430074, P. R. China.
⁴ State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, 102249, P. R. China.
⁵ Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis, School of Chemistry, Cardiff University, Cardiff, CF10 3AT, UK.
⁶ Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, P. R. China.
⁷ National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing, 101408, P. R. China.

PMID: 35347821
DOI: 10.1002/anie.202200763

Abstract

The development of highly active single-atom catalysts (SACs) and identifying their intrinsic active sites in oxidizing industrial hazardous hydrocarbons are challenging prospects. Tuning the electronic metal-support interactions (EMSIs) is valid for modulating the catalytic performance of SACs. We propose that the modulation of the EMSIs in a Pt₁ -CuO SAC significantly promotes the activity of the catalyst in acetone oxidation. The EMSIs promote charge redistribution through the unified Pt-O-Cu moieties, which modulates the d-band structure of atomic Pt sites, and strengthens the adsorption and activation of reactants. The positively charged Pt atoms are superior for activating acetone at low temperatures, and the stretched Cu-O bonds facilitate the activation of lattice oxygen atoms to participate in subsequent oxidation. We believe that this work will guide researchers to engineer efficient SACs for application in hydrocarbon oxidation reactions.

Keywords: Acetone Oxidation; Electronic Metal-Support Interactions; Intrinsic Mechanism; Single-Atom Catalysts.

Abstract

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