Carbon‐Doped BN Nanosheets for the Oxidative Dehydrogenation of Ethylbenzene

Guo, Fangsong; Yang, Pengju; Pan, Zhiming; Cao, Xu‐Ning; Xie, Zailai; Wang, Xinchen

doi:10.1002/ange.201703789

Cited by 80 publications

(36 citation statements)

References 42 publications

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“…8 Recently, our group, followed by others reported that h-BN and BNNTs are surprisingly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins. [9][10][11][12][13][14] For example, propane ODH at 500 °C over h-BN results in 76.0% selectivity to propylene, 11.5% to ethylene and only 9.4% to COx (CO plus CO2) at 19.1% propane conversion. These selectivities result in an olefin yields that are higher than obtained with state-of-theart supported vanadium oxide catalysts 15,16 while achieving good productivity (i.e., 2 kg propene per kg of catalyst per hour).…”

Section: Introductionmentioning

confidence: 99%

Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

et al. 2018

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Hexagonal boron nitride (h-BN) and boron nitride nanotubes (BNNT) were recently reported as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins in the gas phase. Previous studies revealed a substantial increase in surface oxygen content after exposure to ODH conditions (heating to ca. 500 °C under a flow of alkane and oxygen); however, the complexity of these materials has thus far precluded an in-depth understanding of the oxygenated surface species. In this contribution, we combine advanced NMR spectroscopy experiments with scanning electron microscopy and soft X-ray absorption spectroscopy to characterize the molecular structure of the oxygen functionalized phase that arises on h-BN and BNNT following catalytic testing for ODH of propane. The pristine BN materials are readily oxidized and hydrolyzed under ODH reaction conditions to yield a phase consisting of three-coordinate boron sites with variable numbers of hydroxyl and bridging oxide groups which is denoted B(OH)xO3-x (where x = 0-3). Evidence for this robust oxide phase revises previous literature hypotheses of hydroxylated BN edges as the active component on h-BN.

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Section: Introductionmentioning

confidence: 99%

Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

et al. 2018

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“…In recent years, hexagonal boron nitride (h-BN) and other boron-containing (bulk) materials have been reported as highly selective catalysts for the oxidative dehydrogenation (ODH) of light alkanes to olefins. [1][2][3][4][5][6][7][8] For all of these active materials, X-ray photoelectron spectroscopy (XPS) and InfraRed spectroscopy revealed the formation of oxidized boron species on the surface of the materials following catalytic testing for the ODH of propane. [7][8] We recently investigated spent h-BN ODH catalysts using (multidimensional) solid-state NMR spectroscopy, X-ray absorption spectroscopy (XAS), and scanning electron microscopy (SEM).…”

Section: Introductionmentioning

confidence: 99%

Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane

et al. 2019

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In this contribution we report on the oxidative dehydrogenation (ODH) activity of silica-supported boron oxide prepared via incipient wetness impregnation. Characterization of pristine and spent catalysts with infrared, Raman, and solid-state NMR spectroscopy reveals the presence of both isolated and aggregated oxidized boron sites. The results of these investigations, in combination with our earlier work on bulk boron-containing ODH catalysts (e.g., h-BN, metal borides, and elemental boron), bolster the hypothesis that oxidized boron species in situ formed on the surface of these materials are responsible for the exceptional catalytic behavior. We anticipate that investigation of supported boron materials can provide insight into the structural characteristics required for selective boron-containing ODH catalysts. Disciplines DisciplinesPhysical Chemistry Comments CommentsAbstract. In this contribution we report on the oxidative dehydrogenation (ODH) activity of silica-supported boron oxide prepared via incipient wetness impregnation. Characterization of pristine and spent catalysts with infrared, Raman, and solid-state NMR spectroscopy reveals the presence of both isolated and aggregated oxidized boron sites. The results of these investigations, in combination with our earlier work on bulk boron-containing ODH catalysts (e.g., h-BN, metal borides, and elemental boron), give direct evidence that oxidized boron species formed in situ on the surface of these materials are responsible for the exceptional catalytic behavior. We anticipate that investigation of supported boron materials can provide insight into the structural characteristics required for selective boron-containing ODH catalysts.

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“…Introduction of graphene domain also facilitates the electron transportation process, and BCN materials could impart carbon catalysis to BN materials for several catalytic applications with notable activity enhancement (16,17). For example, BCN nanosheets exhibit both high activity and excellent oxidation resistance in ODH of ethylbenzene to styrene (18), as well as notable catalytic activity for oxygen reduction (19). However, the catalytic applications of BCN materials are still at an early proof of concept stage (20), and the molecular design and synthesis of BCN catalysts and quantification of the catalytic activity of each functionality remain to be explored (21).…”

Section: Introductionmentioning

confidence: 99%

Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites

Zhang

Yan

et al. 2020

Sci. Adv.

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Borocarbonitrides (BCNs) have emerged as highly selective catalysts for the oxidative dehydrogenation (ODH) reaction. However, there is a lack of in-depth understanding of the catalytic mechanism over BCN catalysts due to the complexity of the surface oxygen functional groups. Here, BCN nanotubes with multiple active sites are synthesized for oxygen-assisted methanol conversion reaction. The catalyst shows a notable activity improvement for methanol conversion (29%) with excellent selectivity to formaldehyde (54%). Kinetic measurements indicate that carboxylic acid groups on BCN are responsible for the formation of dimethyl ether, while the redox catalysis to formaldehyde occurs on both ketonic carbonyl and boron hydroxyl (B─OH) sites. The ODH reaction pathway on the B─OH site is further revealed by in situ infrared, x-ray absorption spectra, and density functional theory. The present work provides physical-chemical insights into the functional mechanism of BCN catalysts, paving the way for further development of the underexplored nonmetallic catalytic systems.

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Carbon‐Doped BN Nanosheets for the Oxidative Dehydrogenation of Ethylbenzene

Cited by 80 publications

References 42 publications

Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane

Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites

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