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“Borosilicate Zeolite Enriched in Defect Boron Sites Boosting the Low Temperature Oxidative Dehydrogenation of Propane”
被 J. Catal 接受发表!
Bin Qiu, Wen-Duo Lu, Xin-Qian Gao, Jian Sheng, Bing Yan, Min Ji, An-Hui Lu*. Borosilicate Zeolite Enriched in Defect Boron Sites Boosting the Low Temperature Oxidative Dehydrogenation of Propane. J. Catal., 2022, Accepted. [DOWNLOAD]

Abstract
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 golefin gcat-1 h-1 under low reaction temperature (445 ºC) and high weight-hour-space-velocity (WHSV, 37.6 gC3H8 gcat-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 hydrogen bond with adjacent Si−OH groups are identified as the active center and high efficiency in catalyzing ODHP reaction at low temperature.