Abstract
In this paper, Pd/C catalysts are synthesized via Ar glow-discharge plasma reduction using activated carbon as the support and Pd(acac)2, Pd(NO3)2, K2PdCl4, and H2PdCl4 as the Pd precursors, and their catalytic performances are investigated by hydrogen production from dodecahydro-N-ethylcarbazole (H12-NEC). Pd/C-A, prepared from Pd(acac)2, which has the smallest palladium nanoparticles (1.7 nm), the highest dispersion (34%) and no residue of inorganic ions, exhibits the best catalytic activity with a hydrogen release of 5.28 wt.%, which is 2.2 times that of Pd/C-H. The order of the apparent activation energies of the prepared Pd/C catalysts, according to the kinetics of the H12-NEC dehydrogenation reaction, is as follows: Pd/C-A ≈ Pd/C-N < Pd/C-K < Pd/C-H. When Pd(acac)2 with a large ligand acts as a cation Pd precursor, the effect of coulombic attraction to Pd2+ during the plasma reduction process makes it difficult for Pd nanoparticles (NPs) to migrate, which leads to the formation of ultrafine Pd NPs.
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The datasets used and analyzed during the current study are available from the corresponding author on reasonable request.
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This work was supported by the National Key R&D Program (2018YFE0108800), the National Natural Science Foundation of China (21676074), and the Science Foundation of Heilongjiang Academy of Sciences (KY2020SH01).
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All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by Zhaolu Feng, Xiaomin Chen, and Xuefeng Bai. The first draft of the manuscript was written by Zhaolu Feng and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Conceptualization: Xuefeng Bai and Zhaolu Feng; Methodology: Zhaolu Feng; Formal analysis and investigation: Zhaolu Feng; Writing - original draft preparation: Zhaolu Feng; Writing—review and editing: Xuefeng Bai; Funding acquisition: Xuefeng Bai; Resources: Xuefeng Bai; Supervision: Xuefeng Bai and Xiaomin Chen.
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Feng, Z., Chen, X. & Bai, X. Hydrogen production from the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole: effect of Pd precursor on the catalytic performance of Pd/C catalysts. Environ Sci Pollut Res 28, 61623–61635 (2021). https://doi.org/10.1007/s11356-021-15108-6
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DOI: https://doi.org/10.1007/s11356-021-15108-6