TY - JOUR
T1 - Facile construction of Cu(I)Y zeolite via olefin-mediated reduction for separation of olefin/paraffin
AU - He, Wen Jun
AU - Shen, Jia Xin
AU - Zhang, Kai Bo
AU - Qi, Shi Chao
AU - Li, Yu Xia
AU - Zhao, Jing
AU - Sun, Lin Bing
N1 - Publisher Copyright:
© 2025 Elsevier B.V.
PY - 2025/8/30
Y1 - 2025/8/30
N2 - 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.
AB - 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.
KW - Adsorption
KW - CH/CH separation
KW - Cu(II) reduction
KW - Cuprous species
KW - π-complexation
UR - http://www.scopus.com/inward/record.url?scp=86000804606&partnerID=8YFLogxK
U2 - 10.1016/j.seppur.2025.132553
DO - 10.1016/j.seppur.2025.132553
M3 - 文章
AN - SCOPUS:86000804606
SN - 1383-5866
VL - 364
JO - Separation and Purification Technology
JF - Separation and Purification Technology
M1 - 132553
ER -