Generation of Cu(I) Sites in Y Zeolite via In Situ Ethylene Reduction for Ethylene/Ethane Separation

作者：Wen-Jun He, Jiaxin Shen, KaiBo Zhang, Shi‐Chao Qi, Jing Zhao, Yuxia Li, Lin-Bing Sun · 发表于：Industrial & Engineering Chemistry Research · 年份：2026 · DOI：10.1021/acs.iecr.5c04815 · 研究领域：Zeolite Catalysis and Synthesis、Catalytic Processes in Materials Science、Metal-Organic Frameworks: Synthesis and Applications

Ethylene (C 2 H 4 ) serves as a core petrochemical feedstock, but its separation from ethane (C 2 H 6 ) is energy-intensive due to their nearly identical molecular diameters and closely matched boiling points. Cu(I)-based adsorbents offer a solution by selectively capturing C 2 H 4 through π-complexation, delivering a superior separation performance compared to traditional methods. However, conventional Cu(I)-based adsorbents preparation typically relies on high-temperature self-reduction (HTSR, ≥450 °C), resulting in high energy consumption but low Cu(I) yield. In this study, we present an in situ C 2 H 4 reduction (IER) strategy to selectively convert Cu(II) in Y zeolite to Cu(I) at a much lower temperature of 170 °C under a flowing C 2 H 4 atmosphere. The obtained CuY-170 adsorbent achieved an impressive 84.5% Cu(I) yield, obviously outperforming the HTSR method. Density functional theory (DFT) calculations indicate that the IER strategy reduces the reduction energy barrier from 510 kJ mol –1 in the HTSR method to 362 kJ mol –1, thus reducing the energy consumption. Benefiting from the abundant Cu(I) sites, CuY-170 demonstrates a C 2 H 4 adsorption capacity of 4.27 mmol g –1 and a C 2 H 4 /C 2 H 6 selectivity of 41.2, far surpassing previously reported Cu-containing adsorbents, such as CuCl/NaX (1.90 mmol g –1, selectivity 3.6), 1.5 CuCoM-DS (2.25 mmol g –1, selectivity 2.6), and Cu-MCM-48 (0.50 mmol g –1, selectivity 3.8). Moreover, CuY-170 maintains a high C 2 H 4 adsorp...