TY - JOUR
T1 - Engineering of PtZn@S-1 Using an Alkali-Acid Pair Strategy
T2 - Applied for Ethane Dehydrogenation
AU - Zhang, Linlong
AU - Tian, Jingqing
AU - Liu, Ruiqiang
AU - Ma, Bing
AU - Zhao, Chen
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025/7/4
Y1 - 2025/7/4
N2 - Developing synthetic strategies for high-quality metal-zeolite composites is critical for achieving advanced catalytic performances. One major challenge lies in addressing the rate mismatch between rapid metal deposition and slow zeolite crystallization, which leads to the segregation of large metal particles. Herein, we propose a universal strategy via quaternary ammonium alkali-metallic acid (QAMA) pairs for fabricating highly dispersed metal@zeolite materials with nearly 100% metal (Ru, Ir, Pd, Pt, and Zn) utilization. Using tetrapropylammonium hydroxide (TPAOH) as both a structural-directing agent and basic medium, the interaction of TPA+ with acidic metal precursors forms the “QAMA” pairs, which inhibit the precipitation of metal precursors and guide their dispersion into the 10-membered ring channels of MFI topology. Furthermore, the appropriate Si-OH groups on the silicalite-1 (S-1) seeds surface anchor the “QAMA” pairs and thus assist in the subnanometer PtZn particle dispersion. A series of PtZn@S-1 catalysts exhibited outstanding catalytic activity (14.1 molC2H4·gPt-1·h-1 at 24 h-1 weight hourly space velocity (WHSV)) and stability (Kd = 0.0004 h-1) in ethane dehydrogenation (EDH), particularly at relatively low temperature (550 °C) with pure ethane feed.
AB - Developing synthetic strategies for high-quality metal-zeolite composites is critical for achieving advanced catalytic performances. One major challenge lies in addressing the rate mismatch between rapid metal deposition and slow zeolite crystallization, which leads to the segregation of large metal particles. Herein, we propose a universal strategy via quaternary ammonium alkali-metallic acid (QAMA) pairs for fabricating highly dispersed metal@zeolite materials with nearly 100% metal (Ru, Ir, Pd, Pt, and Zn) utilization. Using tetrapropylammonium hydroxide (TPAOH) as both a structural-directing agent and basic medium, the interaction of TPA+ with acidic metal precursors forms the “QAMA” pairs, which inhibit the precipitation of metal precursors and guide their dispersion into the 10-membered ring channels of MFI topology. Furthermore, the appropriate Si-OH groups on the silicalite-1 (S-1) seeds surface anchor the “QAMA” pairs and thus assist in the subnanometer PtZn particle dispersion. A series of PtZn@S-1 catalysts exhibited outstanding catalytic activity (14.1 molC2H4·gPt-1·h-1 at 24 h-1 weight hourly space velocity (WHSV)) and stability (Kd = 0.0004 h-1) in ethane dehydrogenation (EDH), particularly at relatively low temperature (550 °C) with pure ethane feed.
KW - dry-gel conversion
KW - ethane dehydrogenation
KW - heterogeneous catalysis
KW - metal@zeolite
KW - targeted encapsulation
UR - https://www.scopus.com/pages/publications/105007987775
U2 - 10.1021/acscatal.5c02402
DO - 10.1021/acscatal.5c02402
M3 - 文章
AN - SCOPUS:105007987775
SN - 2155-5435
VL - 15
SP - 10971
EP - 10981
JO - ACS Catalysis
JF - ACS Catalysis
IS - 13
ER -