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Acetylene hydrochlorination using porphyrin boosted Cu/AC catalysts with low loading

•0.5CuTPP/AC exhibits excellent performance comparable to high loading Cu catalysts.•TPP ligands control the Cu species dispersion and induce CuN4 single-atom sites.•The co-existence of E-R and L-H reaction pathways ensures the durability of CuTPP/AC. The constraining relationships between Cu-based...

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Bibliographic Details
Published in:Molecular catalysis 2025-02, Vol.572, Article 114756
Main Authors: Zhang, Haifeng, Zhang, Zilong, Zuo, Fangmin, Meng, Yushun, Yang, Liyong, Cai, Tianzi, Huang, Xubin, Du, Yuhui, Wang, Weixue, Wang, Bolin, Yue, Yuxue
Format: Article
Language:English
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Summary:•0.5CuTPP/AC exhibits excellent performance comparable to high loading Cu catalysts.•TPP ligands control the Cu species dispersion and induce CuN4 single-atom sites.•The co-existence of E-R and L-H reaction pathways ensures the durability of CuTPP/AC. The constraining relationships between Cu-based catalyst ligands and catalytic performance need to be elucidated. Herein, activated carbon (AC) supported Cu-based catalyst stabilized by tetraphenylporphyrin (TPP) ligands are constructed and evaluated in acetylene hydrochlorination. The developed 0.5 wt.% CuTPP/AC catalyst exhibits outstanding performance comparable to highly loaded copper-based catalysts. Detailed characterisations and density functional theory (DFT) calculations indicate that the addition of TPP ligands controlled the dispersion of Cu species and induced the generation of highly active CuN4 single-atom sites, and thereby governs the aforementioned activity gap. Diversified reaction pathways of Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) are coexisted owing to the minimal activation energy difference of 0.2 eV, which ensures the durability of CuTPP/AC catalyst. The developed extremely low loading Cu-based catalyst provides necessary potential for industrial applications. [Display omitted]
ISSN:2468-8231
2468-8231
DOI:10.1016/j.mcat.2024.114756