Direct identification of the carbonate intermediate during water-gas shift reaction at Pt-NiO interfaces using surface-enhanced Raman spectroscopy

doi:10.1016/S1872-2067(21)63964-5

Abstract

Abstract:

Noble metal-reducible oxide interfaces have been regarded as one of the most active sites for water-gas shift reaction. However, the molecular reaction mechanism of water-gas shift reaction at these interfaces still remains unclear. Herein, water-gas shift reaction at Pt-NiO interfaces has been in-situ explored using surface-enhanced Raman spectroscopy by construction of Au@Pt@NiO nanostructures. Direct Raman spectroscopic evidence demonstrates that water-gas shift reaction at Pt-NiO interfaces proceeds via an associative mechanism with the carbonate species as a key intermediate. The carbonate species is generated through the reaction of adsorbed CO with gaseous water, and its decomposition is a slow step in water-gas shift reaction. Moreover, the Pt-NiO interfaces would promote the formation of this carbonate intermediate, thus leading to a higher activity compared with pure Pt. This spectral information deepens the fundamental understanding of the reaction mechanism of water-gas shift reaction, which would promote the design of more efficient catalysts.

Key words: Water-gas shift reaction, Surface-enhanced Raman spectroscopy, Core-shell nanostructure, In-situ characterization, Carbonate intermediate

Si-Na Qin, Di-Ye Wei, Jie Wei, Jia-Sheng Lin, Qing-Qi Chen, Yuan-Fei Wu, Huai-Zhou Jin, Hua Zhang, Jian-Feng Li. Direct identification of the carbonate intermediate during water-gas shift reaction at Pt-NiO interfaces using surface-enhanced Raman spectroscopy[J]. Chinese Journal of Catalysis, 2022, 43(8): 2010-2016.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63964-5

https://www.cjcatal.com/EN/Y2022/V43/I8/2010

Figures/Tables 4

Fig. 1. (a) Illustration of Au@Pt@NiO nanostructures and in-situ SERS study of WGSR at Pt-NiO interfaces. (b) TEM images of Au@Pt@NiO. (c) HAADF-STEM image and elemental maps of Au@Pt@NiO.

Fig. 2. (a) In-situ SERS spectra of CO adsorbed on the Au@NiO, Au@Pt, Au@Pt@NiO. Au@Pt@NiO-thin and Au@Pt@NiO-thick mean the Au@Au@Pt@NiO nanoparticles using 0.05 and 0.5 mL nickel precursors, respectively. (b) In-situ SERS spectra for WGSR over Au@Pt@NiO. (c) Normalized peak intensity of the 1065 cm-1 band and Pt-C band as a function of reaction temperature. The blue curve is the catalytic performance of WGSR.

Fig. 3. (a) In-situ SERS spectra for WGSR over Au@Pt NPs at the atmospheres of CO/H2O = 1/2. In-situ SERS spectra of Au@Pt@NiO NPs at the atmosphere of Ar (b), CO (c), H2O (d) alone.

Fig. 4. (a,c) In-situ SERS spectra of WGSR at Au@Pt@NiO under atmosphere switching conditions. (a) CO is first adsorbed at Au@Pt@NiO at room temperature, then the gas is changed to 2% H2O/Ar and the temperature is raised. (c) Au@Pt@NiO is first kept under 2% H2O/Ar, then the gas is changed to 1% CO and the temperature is raised. (b) Corresponding normalized intensity of the Raman bands for the adsorbed carbonate and CO species in (a) as a function of temperature. (d) Schematic of the proposed reaction mechanism WGSR at Pt-NiO interfaces.

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