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/anie.201703789

Cited by 204 publications

(93 citation statements)

References 44 publications

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“…Boron‐containing materials, such as hexagonal boron nitride and boron nitride nanotubes, have been shown to be highly selective catalysts for the transformation of light alkanes to olefins via oxidative dehydrogenation (ODH) . Analysis of these materials after catalytic testing for the ODH of propane revealed the formation of an oxidized, amorphous boron phase at the catalyst surface.…”

Section: Figurementioning

confidence: 93%

B‐MWW Zeolite: The Case Against Single‐Site Catalysis

et al. 2020

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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 B2(OH)xO(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 11B 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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Section: Figurementioning

confidence: 93%

B‐MWW Zeolite: The Case Against Single‐Site Catalysis

et al. 2020

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“…sheds light on the possibility for the replacement and upgrade of conventional metal‐based catalytic systems to meet the urgent demands of green and sustainable chemical engineering process in modern society. The unique and intriguing catalytic property of non‐metallic carbon materials, for example the relatively high selectivity in alkane oxidative dehydrogenation reaction (ODH), provides carbon‐related materials great potential in catalysis. However, comparing with the rapid development of novel carbon material synthesis and new carbon catalytic reaction systems, the research progress of the mechanisms of carbon catalytic reactions is pretty slow, which seriously restricts the establishment of the fundamental theory of the carbon catalysis and the rational design of the efficient carbon catalytic reaction systems .…”

Section: Figurementioning

confidence: 99%

Oxidative Dehydrogenation on Nanocarbon: Revealing the Reaction Mechanism via In Situ Experimental Strategies

et al. 2018

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Classical mechanistic analysis strategy, including active site chemical titration, kinetic measurement and corresponding isotopic effect and surface reaction of single reactant etc., were performed in oxidative dehydrogenation reactions on nanocarbon. The detailed reaction mechanism for non‐metallic carbon catalytic process was revealed via in situ experimental methods, which sheds light on the accurate quantitative description and structure‐function relations for carbon catalysis.

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“…By contrast, metal‐free graphene oxide and graphitic carbon nitride (g‐CN) polymer, comprising earth‐abundant elements such as C, N, and O, exhibited high photocatalytic activity for H 2 production from aqueous solutions. Its ecofriendly chemical composition and ease of synthesis make g‐CN a promising substitute for ceramic photocatalysts . Developing a structural design of g‐CN to enhance absorption in the solar spectrum, facilitate separation of photogenerated charges, and expose the active sites for charge transfer is a major challenge for improving the applicability of g‐CN.…”

Section: Introductionmentioning

confidence: 99%

Oligomer‐Incorporated Polymeric Layer Framework of Graphitic Carbon Nitride for Effective Photocatalytic Hydrogen Evolution

Huang

Teng

2017

Part & Part Syst Charact

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Developing a structural design of g-CN to enhance absorption in the solar spectrum, [11] facilitate separation of photogenerated charges, [12] and expose the active sites for charge transfer [13] is a major challenge for improving the applicability of g-CN.The structure of g-CN comprises 2D layers that are constituted by H-bondingconnected melon strains (Scheme 1). [14] The layers are linked through van der Waals attraction to form a 3D framework. Scheme 1 elucidates that the melon strain is produced through polymerization of 1,3,4,6,7,9,9b-Heptaazaphenalene-2,5,8-triamine (melem) molecules along with NH 3 removal; its structure comprises heptazine units connected by NH bridges. This g-CN framework results in an electronic structure exhibiting a bandgap straddling the redox potentials for H 2 and O 2 evolutions from water splitting and a gap width of ≈2.7 eV, [4] which enables g-CN to capture a considerable amount of solar irradiation.Previous studies have reported that crystalline graphite-like CN (i.e., g-C 3 N 4 ) exhibited negligible activity in photocatalysis, whereas g-CN, which is partially condensed and contains amino groups, was active in H 2 evolution under illumination. [15] Lotsch and co-workers reported that low-molecular-weight melon, a type of melem oligomer, exhibited a higher efficiency than melon in H 2 evolution under illumination at λ ≈ 420 nm. This was because of the increase in kinetics even though the energy gap of the melem oligomer was larger than that of melon. [16] Theoretical calculations have indicated that the lowest unoccupied molecular orbital of melem oligomers is contributed by hybrid systems comprising edged carbon and nitrogen atoms, central nitrogen atoms, and bridging amino groups, and by localized terminal primary amines. [16,17] Experimental studies on dendrimers and metal-organic frameworks have revealed that photodeposition of metallic platinum in H 2 PtCl 6 solution preferentially occurred at the amino groups. [18] These findings imply that the amino groups of melem oligomers acted as the electron-donating sites for photocatalytic H 2 evolution and their robust interaction with the deposited metallic platinum facilitated the transfer of excited electrons from the amino sites to the solution phase for H 2 evolution. [19] A framework comprising melem oligomers for providing amino sites can enable the production of g-CN materials with high photocatalytic activity. [13,20] However, melem oligomers are wide-bandgap This paper presents a structural design of graphitic carbon nitride (CN) for use as an active photocatalyst in H 2 evolution reactions. The active photocatalyst is synthesized by subjecting a CN sample to consecutive annealing and ammonia treatments. The CN sample is produced through urea condensation. The annealing treatment destroys the polymeric CN to form a defective polymeric layer framework incorporating 1,3,4,6,7,9,9b-Heptaazaphenalene-2,5,8-triamine (melem) oligomers. The annealed CN exhibits a wide absorption range in visible light because the distorted ...

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Carbon‐Doped BN Nanosheets for the Oxidative Dehydrogenation of Ethylbenzene

Cited by 204 publications

References 44 publications

B‐MWW Zeolite: The Case Against Single‐Site Catalysis

B‐MWW Zeolite: The Case Against Single‐Site Catalysis

Oxidative Dehydrogenation on Nanocarbon: Revealing the Reaction Mechanism via In Situ Experimental Strategies

Oligomer‐Incorporated Polymeric Layer Framework of Graphitic Carbon Nitride for Effective Photocatalytic Hydrogen Evolution

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