High-temperature reactivity of vanadium oxide clusters in methane activation: Vibrational degrees of freedom matter

Author:

Ruan Man123,Zhao Yan-Xia13ORCID,Wei Gong-Ping123,He Sheng-Gui123ORCID

Affiliation:

1. State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences 1 , Beijing 100190, People’s Republic of China

2. University of Chinese Academy of Sciences 2 , Beijing 100049, People’s Republic of China

3. Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences 3 , Beijing 100190, People’s Republic of China

Abstract

Understanding the properties of small particles working under high-temperature conditions at the atomistic scale is imperative for exact control of related processes, but it is quite challenging to achieve experimentally. Herein, benefitting from state-of-the-art mass spectrometry and by using our newly designed high-temperature reactor, the activity of atomically precise particles of negatively charged vanadium oxide clusters toward hydrogen atom abstraction (HAA) from methane, the most stable alkane molecule, has been measured at elevated temperatures up to 873 K. We discovered the positive correlation between the reaction rate and cluster size that larger clusters possessing greater vibrational degrees of freedom can carry more vibrational energies to enhance the HAA reactivity at high temperature, in contrast with the electronic and geometric issues that control the activity at room temperature. This finding opens up a new dimension, vibrational degrees of freedom, for the simulation or design of particle reactions under high-temperature conditions.

Funder

National Natural Science Foundation of China

Youth Innovation Promotion Association of the Chinese Academy of Sciences

Publisher

AIP Publishing

Subject

Physical and Theoretical Chemistry,General Physics and Astronomy

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