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Unveiling the Mechanism of Plasma-Catalytic Low-Temperature Water–Gas Shift Reaction over Cu/γ-Al<sub>2</sub>O<sub>3</sub> Catalysts

Xiaoqiang Shen, Michael Craven, Jiacheng Xu, Yaolin Wang, Zhi Li, Weitao Wang, Shuiliang Yao, Zuliang Wu, Nan Jiang, Xuanbo Zhou, Kuan Sun, Xuesen Du, Xin Tu

2024JACS Au20 citationsDOIOpen Access PDF

Abstract

High Resolution Image Download MS PowerPoint Slide The water–gas shift (WGS) reaction is a crucial process for hydrogen production. Unfortunately, achieving high reaction rates and yields for the WGS reaction at low temperatures remains a challenge due to kinetic limitations. Here, nonthermal plasma coupled to Cu/γ-Al 2 O 3 catalysts was employed to enable the WGS reaction at considerably lower temperatures (up to 140 °C). For comparison, thermal-catalytic WGS reactions using the same catalysts were conducted at 140–300 °C. The best performance (72.1% CO conversion and 67.4% H 2 yield) was achieved using an 8 wt % Cu/γ-Al 2 O 3 catalyst in plasma catalysis at ∼140 °C, with 8.74 MJ mol –1 energy consumption and 8.5% H 2 fuel production efficiency. Notably, conventional thermal catalysis proved to be ineffective at such low temperatures. Density functional theory calculations, coupled with in situ diffuse reflectance infrared Fourier transform spectroscopy, revealed that the plasma-generated OH radicals significantly enhanced the WGS reaction by influencing both the redox and carboxyl reaction pathways.

Topics & Concepts

Water-gas shift reactionCatalysisPlasmaReaction mechanismMaterials scienceChemistryPhysicsOrganic chemistryQuantum mechanicsCatalytic Processes in Materials ScienceCatalysts for Methane ReformingAmmonia Synthesis and Nitrogen Reduction