B–MWW Zeolite: The Case Against Single–Site Catalysis
Abstract
Abstract 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 11 B solid‐state NMR spectroscopy, we show that the majority of boron species in B‐MWW exist as isolated BO 3 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 BO 3 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.
- Authors:
-
[1];
[1]
- Univ. of Wisconsin, Madison, WI (United States)
- Ames Lab., and Iowa State Univ., Ames, IA (United States)
- Iowa State Univ., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Univ. of Wisconsin, Madison, WI (United States)
- Sponsoring Org.:
- USDOE; National Science Foundation (NSF); National Institutes of Health (NIH)
- OSTI Identifier:
- 1866351
- Alternate Identifier(s):
- OSTI ID: 1602080
- Grant/Contract Number:
- SC0017918; AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 16; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; zeolites; boron; heterogeneous catalysis; oxidative dehydrogenation; solid-state NMR
Citation Formats
Altvater, Natalie R., Dorn, Rick W., Cendejas, Melissa C., McDermott, William P., Thomas, Brijith, Rossini, Aaron J., and Hermans, Ive. B–MWW Zeolite: The Case Against Single–Site Catalysis. United States: N. p., 2020.
Web. doi:10.1002/anie.201914696.
Altvater, Natalie R., Dorn, Rick W., Cendejas, Melissa C., McDermott, William P., Thomas, Brijith, Rossini, Aaron J., & Hermans, Ive. B–MWW Zeolite: The Case Against Single–Site Catalysis. United States. https://doi.org/10.1002/anie.201914696
Altvater, Natalie R., Dorn, Rick W., Cendejas, Melissa C., McDermott, William P., Thomas, Brijith, Rossini, Aaron J., and Hermans, Ive. Wed .
"B–MWW Zeolite: The Case Against Single–Site Catalysis". United States. https://doi.org/10.1002/anie.201914696. https://www.osti.gov/servlets/purl/1866351.
@article{osti_1866351,
title = {B–MWW Zeolite: The Case Against Single–Site Catalysis},
author = {Altvater, Natalie R. and Dorn, Rick W. and Cendejas, Melissa C. and McDermott, William P. and Thomas, Brijith and Rossini, Aaron J. and Hermans, Ive},
abstractNote = {Abstract 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 11 B solid‐state NMR spectroscopy, we show that the majority of boron species in B‐MWW exist as isolated BO 3 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 BO 3 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.},
doi = {10.1002/anie.201914696},
journal = {Angewandte Chemie (International Edition)},
number = 16,
volume = 59,
place = {United States},
year = {Wed Feb 05 00:00:00 EST 2020},
month = {Wed Feb 05 00:00:00 EST 2020}
}
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