Borosilicate zeolite enriched in defect boron sites boosting the low-temperature oxidative dehydrogenation of propane

被引:32
作者
Qiu, Bin [1 ]
Lu, Wen -Duo [1 ]
Gao, Xin-Qian [1 ]
Sheng, Jian [1 ]
Yan, Bing [1 ]
Ji, Min [1 ]
Lu, An -Hui [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Liaoning Key Lab Catalyt Convers Carbon Resources, Dalian 116024, Liaoning, Peoples R China
关键词
Boron species; Coordination environment; Dynamic evolution; ODHP; Propylene; SILICA-SUPPORTED BORON; HIGH SELECTIVITY; OXIDE CATALYSTS; ETHANE; CRYSTALS; OLEFINS;
D O I
10.1016/j.jcat.2022.02.017
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Borosilicate zeolites are the active catalysts in oxidative dehydrogenation of propane (ODHP), which provide an ideal platform to explore the origin of catalytic activity for boron-containing catalysts as well as the construction of highly active boron centers. Herein, we report that the incompletely crystallized MFI-type borosilicate zeolite catalyst displays extraordinary performance in ODHP, exhibiting an olefin productivity of 4.75 g(olefin) g(cat)(-1) h(-1) under low reaction temperature (445 & DEG;C) and high weight-hour-space-velocity (WHSV, 37.6 gC(3H8) g(cat)(-1) h(-1)). A combination of solid-state NMR, dual-beam FTIR, and in-situ DRIFT measurements reveal that the boron species are anchored to the zeolite matrix in the form of open coordination. Meanwhile, the ample Si-OH groups on the surface facilitate the formation of hydrogen bonds with the B-OH in defective boron species and inhibit the excessive leaching of boron. During the ODHP process, the isolated boron species would dynamically transform into aggregated ones, being closely related to the increased catalytic activity. The B-OH groups in aggregated BOx species that hydro-gen bond with adjacent Si-OH groups are identified as the active center and high efficiency in catalyzing ODHP reaction at low temperature. (C) 2022 Elsevier Inc. All rights reserved.
引用
收藏
页码:133 / 141
页数:9
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