Enhancing the Reaction of CO2 and H2O Using Catalysts within a Nonthermal Plasma

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-04-16 DOI:10.1021/acscatal.5c00747

Piu Chawdhury, Sarayute Chansai, Matthew Conway, Joseph Parker, Matthew Lindley, Cristina E. Stere, Meenakshisundaram Sankar, Sarah J. Haigh, Ben Dennis-Smither, Sorin V. Filip, Stephen Poulston, Peter Hinde, Christopher Hawkins, Christopher Hardacre

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Abstract

The direct conversion of emitted and captured carbon dioxide into usable fuels remains a significant challenge and is a key element in the transition to net zero. Herein, we examine the reaction of CO₂ and H₂O over Ni- and Cu-based catalysts combined with nonthermal plasma (NTP) technology. The catalysis under NTP conditions enabled significantly higher CO₂ conversion and product yield, which was almost six times higher than that of the plasma-only system. A maximum H₂ concentration of ∼2500 ppm was achieved for the Cu/ZSM5 catalyst at 17% CO₂ conversion. Comprehensive catalyst characterization together with the reaction performances reveals that Cu in a reduced state promotes both the CO₂ and H₂O conversion leading to H₂ formation. In situ diffuse reflectance infrared spectroscopy (DRIFTS) coupled with mass spectrometry (MS) analysis of the gas phase products confirms that CO is the major active species to drive the water gas shift reaction to form H₂ in addition to the direct CO₂ and H₂O interaction. It also explains how the different metal support interactions influence the CO adsorption and its interaction with water. Among the catalysts studied, ZSM5-supported Cu catalysts were found to be the most effective in facilitating the CO₂ and H₂O reaction to produce H₂.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.