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Application of coverage-dependent micro-kinetic study to investigate direct H2O2 synthesis mechanism on Pd(111) surface

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Abstract

Hydrogen peroxide (H2O2) is a highly effective, green oxidant that has been widely used in many chemical industries. Two coverage-dependent models are built in micro-kinetic study and successfully applied to investigate the direct H2O2 synthesis mechanism from hydrogen and oxygen on Pd(111) surface. The computational results from both models show that the selectivity to H2O2 can reach 99%, which takes advantage of the repulsion effects between the adsorbates and O* on the surface. H2O2 comes from the sequential hydrogenation of O2 and H2O as the by-product is dominantly from H2O2* decomposition. Therefore, how to inhibit H2O2* decomposition is the key step to achieve high selectivity on Pd(111) surface. Both models show H2O generation with higher apparent activation energy compared to H2O2 formation, indicating that low temperature will benefit selectivity to H2O2. The calculated apparent activation energies are 22.30 kJ mol−1 for H2O2 formation and 48.67 kJ mol−1 for H2O generation by the standard method, which agrees well with the experimental observations. It indicates that the coverage-dependent micro-kinetic study is a feasible method to investigate reaction mechanisms on various surfaces.

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Acknowledgements

We are grateful for financial supports from the Natural Science Foundation of Hebei Province (No. B2017203113, B2016203158) and the National Natural Science Foundation of China (No. 21872136).

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Authors and Affiliations

  1. Hebei Key Laboratory of Applied Chemistry, Hebei Key Laboratory of Heavy Metal Deep-remediation in Water and Resource Reuse, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China

    Keju Sun, Xin Song, Xianfeng Hao & Yuanhui Xu

  2. School of Chemical Engineering and Energy Technology, Dongguan University of Technology, Dongguan, 523808, China

    Hai-Yan Su

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  1. Keju Sun
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  2. Xin Song
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  3. Xianfeng Hao
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Correspondence to Keju Sun.

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Sun, K., Song, X., Hao, X. et al. Application of coverage-dependent micro-kinetic study to investigate direct H2O2 synthesis mechanism on Pd(111) surface. Theor Chem Acc 139, 170 (2020). https://doi.org/10.1007/s00214-020-02676-y

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