Metal‐Free Dehydrogenation of N‐Heterocycles by Ternary <i>h</i>‐BCN Nanosheets with Visible Light

Zheng, Meifang; Shi, Jiale; Tao, Yuan; Wang, Xinchen

doi:10.1002/ange.201800319

Cited by 50 publications

(14 citation statements)

References 81 publications

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“…In addition, these BCN materials have extraordinary properties complementary to those of pure carbon and BN with a wide spectrum of changes in morphology, porosity, surface oxygen functional groups, and electronic structure (15). 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).…”

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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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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“…Furthermore, a probe reaction of the dehydrogenation of 1,2,3,4-tetrahydroquinoline (THQ) reaction was carried out to characterize the dehydrogenation activity for ND and F-ND catalysts (Supplementary Fig. 7 ) 28 . The yield of quinoline for F-ND catalysts is also higher than ND catalysts, illustrating that F-ND catalysts have better dehydrogenation activity, indicating a broad application in dehydrogenation reaction fields 29 .…”

Section: Resultsmentioning

confidence: 99%

Photo-fluorination of nanodiamonds catalyzing oxidative dehydrogenation reaction of ethylbenzene

Luo

Wan

et al. 2021

Nat Commun

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Styrene is one of the most important industrial monomers and is traditionally synthesized via the dehydrogenation of ethylbenzene. Here, we report a photo-induced fluorination technique to generate an oxidative dehydrogenation catalyst through the controlled grafting of fluorine atoms on nanodiamonds. The obtained catalyst has a fabulous performance with ethylbenzene conversion reaching 70% as well as styrene yields of 63% and selectivity over 90% on a stream of 400 °C, which outperforms other equivalent benchmarks as well as the industrial K−Fe catalysts (with a styrene yield of 50% even at a much higher temperature of ca. 600 °C). Moreover, the yield of styrene remains above 50% after a 500 h test. Experimental characterizations and density functional theory calculations reveal that the fluorine functionalization not only promotes the conversion of sp3 to sp2 carbon to generate graphitic layers but also stimulates and increases the active sites (ketonic C=O). This photo-induced surface fluorination strategy facilitates innovative breakthroughs on the carbocatalysis for the oxidative dehydrogenation of other arenes.

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“…[ 89 ] Based on above work, Wang's group find that the ternary h‐BCN can also be used as an efficient metal free photocatalyst in the acceptorless dehydrogenation of N‐heterocycles reactions under visible light. [ 90 ] Due to the wide bandgap, h‐BN is often need to be combined with other materials in a photocatalytic system. Therefore, developing freestanding h‐BN photocatalyst will be regarded as a hot topic in the future research work.…”

Section: Metal Free Thin‐layered Photocatalystmentioning

confidence: 99%

“…Molecular oxygen activation, refers to inert O molecules into highly reactive oxygen‐involved species, such as 1 O 2 , O 2• − , and • OH radicals, is also a kind of widely studied photocatalytic process, which has many application prospects in the field of organic synthesis, pollutants degradation and so on ( Table 4 ). [ 44,48,49,68,77,79,90,91,149,162,168,218–221 ] However, the relative weak interactions between the inert molecular oxygen and the surface of the photocatalysts is the main drawbacks for achieving effective molecular oxygen activation. [ 217 ] In recent years, thin‐layered photocatalysts are considered as good candidates for being applied in the field of molecular oxygen activation.…”

Section: Photocatalytic Applicationsmentioning

confidence: 99%

Thin‐Layered Photocatalysts

Sun

Huang

Zhao

et al. 2020

Adv Funct Materials

132

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Semiconductor photocatalysis, a green and sustainable technology, is of great significance for solving environmental pollution and energy shortages. However, the common problems of inefficient light harvesting, rapid recombination of electron-hole pairs, and low surface reactive reaction sites for photocatalysts urgently need to be solved. In this regard, thin-layered photocatalysts are considered to be one of the most promising candidates for addressing these issues, due to their unique surface and electronic properties. In this review, the various strategies for constructing thin-layered photocatalysts are summarized, and emphasis is given to approaches for optimizing the photocatalytic performance of the thin-layered materials, which can be classified into surface engineering and junction construction. In addition, the photocatalytic applications of thin-layered materials, i.e., water splitting, CO 2 reduction, nitrogen fixation, and molecule oxygen activation, are summarized. Finally, based on current achievements in thin-layered photocatalysts, their future development and challenges are discussed.

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Metal‐Free Dehydrogenation of N‐Heterocycles by Ternary h‐BCN Nanosheets with Visible Light

Cited by 50 publications

References 81 publications

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

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

Photo-fluorination of nanodiamonds catalyzing oxidative dehydrogenation reaction of ethylbenzene

Thin‐Layered Photocatalysts

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