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Density functional theory study of N2O decomposition catalyzed by Pd4−/0/+ clusters

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Abstract

Density functional theory (DFT) is used to investigate the N2O decomposition over Pd4−/0/+ clusters. The Eley–Rideal (ER) mechanism and the Langmuir–Hinshelwood (LH) mechanism are well established. The average binding energies show that the most stable structure of Pd4−/0/+ clusters is the tetrahedral configuration. For the Pd4− cluster, the activation energies indicate that the rate-limiting step in two mechanisms is the formation of O2, and the ER mechanism occurs more easily than the LH mechanism. While for the Pd40 and Pd4+ clusters, the rate-limiting step in two mechanisms is the N2O decomposition to N2, and the LH mechanism is more likely to process. Among all clusters, the Pd4− cluster exhibits better catalytic activity compared with the Pd40 and Pd4+ clusters.

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Acknowledgements

This work is supported by the Science and Technology Research Program of Chongqing Municipal Education Commission (KJQN202101517).

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  1. College of Chemistry and Chemical Engineering, Chongqing University of Science and Technology, Chongqing, 401331, People’s Republic of China

    Xinlin Tang, Wenhong Zeng, Huiyuan Duan, Shuangkou Chen & Xin Lian

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  1. Xinlin Tang
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  2. Wenhong Zeng
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Tang, X., Zeng, W., Duan, H. et al. Density functional theory study of N2O decomposition catalyzed by Pd4−/0/+ clusters. Reac Kinet Mech Cat 136, 1933–1943 (2023). https://doi.org/10.1007/s11144-023-02456-2

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