Plasma-Catalytic CO₂ Hydrogenation over a Pd/ZnO Catalyst: <i>In Situ</i> Probing of Gas-Phase and Surface Reactions

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Sun, Yuhai, Wu, Junliang, Wang, Yaolin ORCID: 0000-0003-1932-9810, Li, Jingjing, Wang, Ni, Harding, Jonathan ORCID: 0000-0002-9920-7831, Mo, Shengpeng, Chen, Limin, Chen, Peirong, Fu, Mingli et al (show 3 more authors) , Ye, Daiqi, Huang, Jun and Tu, Xin ORCID: 0000-0002-6376-0897 (2022) Plasma-Catalytic CO₂ Hydrogenation over a Pd/ZnO Catalyst: <i>In Situ</i> Probing of Gas-Phase and Surface Reactions. JACS AU, 2 (8). pp. 1800-1810.

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Abstract

Plasma-catalytic CO₂ hydrogenation is a complex chemical process combining plasma-assisted gas-phase and surface reactions. Herein, we investigated CO₂ hydrogenation over Pd/ZnO and ZnO in a tubular dielectric barrier discharge (DBD) reactor at ambient pressure. Compared to the CO₂ hydrogenation using Plasma Only or Plasma + ZnO, placing Pd/ZnO in the DBD almost doubled the conversion of CO₂ (36.7%) and CO yield (35.5%). The reaction pathways in the plasma-enhanced catalytic hydrogenation of CO₂ were investigated by <i>in situ</i> Fourier transform infrared (FTIR) spectroscopy using a novel integrated <i>in situ</i> DBD/FTIR gas cell reactor, combined with online mass spectrometry (MS) analysis, kinetic analysis, and emission spectroscopic measurements. In plasma CO₂ hydrogenation over Pd/ZnO, the hydrogenation of adsorbed surface CO₂ on Pd/ZnO is the dominant reaction route for the enhanced CO₂ conversion, which can be ascribed to the generation of a ZnO <i>_x</i> overlay as a result of the strong metal-support interactions (SMSI) at the Pd-ZnO interface and the presence of abundant H species at the surface of Pd/ZnO; however, this important surface reaction can be limited in the Plasma + ZnO system due to a lack of active H species present on the ZnO surface and the absence of the SMSI. Instead, CO₂ splitting to CO, both in the plasma gas phase and on the surface of ZnO, is believed to make an important contribution to the conversion of CO₂ in the Plasma + ZnO system.

Item Type:	Article
Uncontrolled Keywords:	plasma catalysis, CO2 hydrogenation, in situ FTIR, surface reactions, reaction pathways
Divisions:	Faculty of Science and Engineering > School of Electrical Engineering, Electronics and Computer Science
Depositing User:	Symplectic Admin
Date Deposited:	30 Aug 2022 11:33
Last Modified:	17 Oct 2023 14:55
DOI:	10.1021/jacsau.2c00028
Open Access URL:	https://pubs.acs.org/doi/10.1021/jacsau.2c00028
Related URLs:	Author Publisher
URI:	https://livrepository.liverpool.ac.uk/id/eprint/3162305

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• Plasma-Catalytic CO₂ Hydrogenation over a Pd/ZnO Catalyst: <i>In Situ</i> Probing of Gas-Phase and Surface Reactions. (deposited 01 Jun 2022 10:50)
  • Plasma-Catalytic CO₂ Hydrogenation over a Pd/ZnO Catalyst: <i>In Situ</i> Probing of Gas-Phase and Surface Reactions. (deposited 30 Aug 2022 11:33) [Currently Displayed]