Facile construction of Cu(I)Y zeolite via olefin-mediated reduction for separation of olefin/paraffin

Wen Jun He, Jia Xin Shen, Kai Bo Zhang, Shi Chao Qi, Yu Xia Li, Jing Zhao, Lin Bing Sun

科研成果: 期刊稿件文章同行评审

摘要

Ethylene (C2H4) is a central resource for various chemical products, serving as a foundational building block for items like polyethylene and ethylene glycol. However, the efficient separation of C2H4 from ethane (C2H6) poses challenges due to their similar molecular sizes and boiling points. In this context, Cu(I)-bearing adsorbents show significant potential for C2H4/C2H6 separation, as Cu(I) selectively interacts with C2H4 through π-complexation. Nonetheless, the preparation of these adsorbents requires harsh conditions (usually ≥700 °C for over 12 h) to convert Cu(II) species to Cu(I) sites via the traditional self-reduction method, leading to significant energy consumption. This study introduces a mild olefin-mediated reduction method to achieve controlled construction of Cu(I) sites in zeolite Y. Propylene, as a mild reductant, significantly lowers the reduction energy barrier from 510 kJ/mol (under traditional self-reduction) to 332 kJ/mol, allowing for Cu(I) reduction at temperatures below 130 °C for just 2 h. Moreover, the yield of Cu(I) achieved through the olefin-mediated reduction (85.1 %) surpasses that of the high-temperature self-reduction method (≤60 %). Thanks to the abundant Cu(I) sites, the resulting Cu(I)Y-R exhibits an exceptional C2H4 uptake and impressive C2H4/C2H6 selectivity, achieving values of 4.37 mmol/g and 98.31, respectively. This performance surpasses that of various reported adsorbents, including zeolites, mesoporous carbons, and metal–organic frameworks. After five cycles, Cu(I)Y-R maintains its high adsorption capacity, indicating remarkable cyclic stability. This material's remarkable C2H4 uptake and selectivity make it a viable option for effective C2H4/C2H6 separation in industrial settings.

源语言英语
文章编号132553
期刊Separation and Purification Technology
364
DOI
出版状态已出版 - 30 8月 2025

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