期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 16, 页码 6546-6550出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201914696
关键词
boron; heterogeneous catalysis; oxidative dehydrogenation; solid-state NMR; zeolites
资金
- National Science Foundation [CBET-1916809]
- U.S. Department of Energy [DE-SC0017918]
- Ames Laboratory Royalty Account
- Iowa State University
- U.S. DOE [DE-AC02-07CH11358]
- NIH [P41 GM103399, P41GM66326, RR02781, RR08438]
- University of Wisconsin
- NSF [DMB-8415048, OIA-9977486, BIR-9214394]
- USDA
- U.S. Department of Energy (DOE) [DE-SC0017918] Funding Source: U.S. Department of Energy (DOE)
Boron-containing materials have recently been identified as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins. It has previously been demonstrated by several spectroscopic characterization techniques that the surface of these boron-containing ODH catalysts oxidize and hydrolyze under reaction conditions, forming an amorphous B-2(OH)(x)O(3-x/2) (x=0-6) layer. Yet, the precise nature of the active site(s) remains elusive. In this Communication, we provide a detailed characterization of zeolite MCM-22 isomorphously substituted with boron (B-MWW). Using B-11 solid-state NMR spectroscopy, we show that the majority of boron species in B-MWW exist as isolated BO3 units, fully incorporated into the zeolite framework. However, this material shows no catalytic activity for ODH of propane to propene. The catalytic inactivity of B-MWW for ODH of propane falsifies the hypothesis that site-isolated BO3 units are the active site in boron-based catalysts. This observation is at odds with other traditionally studied catalysts like vanadium-based catalysts and provides an important piece of the mechanistic puzzle.
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