Issue 7, 2023

Strong Ruδ+–Ce3+ electronic interaction induced by a CeOy overlayer for enhanced low-temperature N2-to-NH3 conversion

Abstract

Ammonia (NH3) synthesis with hydrogen (H2) produced from renewable energy is a promising route to reduce carbon footprints and the dependence on fossil fuels. However, the development of highly efficient and stable catalyst for NH3 synthesis under mild conditions is a challenge. Herein, a series of boron nitride (BN)-supported Ru catalysts were synthesized, and the NH3 synthesis rate was enhanced significantly after the introduce of Ce. The developed RuCe2.4/BN catalyst with a Ce/Ru molar ratio of 2.4 exhibited the optimal NH3 synthesis rate of 14.6 mmolNH3 gcat−1 h−1 at 400 °C and 1.0 MPa, which was ∼21-fold that of the catalyst prepared without Ce. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and X-ray photoemission spectroscopy coupled with electron energy loss spectroscopy revealed that the d–d electronic interaction between Ru and CeO2 can be differentially adjusted by a change in the Ce/Ru molar ratio. An appropriate amount of Ce could enhance the electronic interaction between the CeOy overlayer and Ru entities. Also, the CeOy overlayer acted as an “electron shuttle” and enhanced the charge transfer from Ce to the surface of Ru atoms. Finally, electron donation occurred from the surface abundancy of Ru atoms to N2 molecule through a d–π* interaction. Moreover, the introduction of excessive Ce could block Ru active sites, weaken the electron transfer and, therefore, decrease the NH3 synthesis rate.

Graphical abstract: Strong Ruδ+–Ce3+ electronic interaction induced by a CeOy overlayer for enhanced low-temperature N2-to-NH3 conversion

Supplementary files

Article information

Article type
Paper
Submitted
29 Nov 2022
Accepted
29 Jan 2023
First published
30 Jan 2023

Catal. Sci. Technol., 2023,13, 2134-2141

Strong Ruδ+–Ce3+ electronic interaction induced by a CeOy overlayer for enhanced low-temperature N2-to-NH3 conversion

L. Li, M. Zhang, T. Zhang, Y. Gao, J. Ni, Y. Zhou, J. Lin, X. Wang and L. Jiang, Catal. Sci. Technol., 2023, 13, 2134 DOI: 10.1039/D2CY02041F

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