<i>N-</i>Oxyl Radicals Trapped on Zeolite Surface Accelerate Photocatalysis

Ma, Runyuan; Chen, Wei; Wang, Qianqian; Yi, Xiaoyan; Xiao, Yao; Gao, Xinhua; Zhang, Jian; Tang, Xiaomin; Yang, Chengguang; Meng, Xiangju; Zheng, Anmin; Xiao, Feng‐Shou

doi:10.1021/acscatal.9b03737

Cited by 18 publications

(26 citation statements)

References 35 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…Their combined XRD, UV–vis DRS, and ESR investigations revealed that photocatalytic activity is related to the content of iron-impurity, irrespective of zeolite properties. Under photoirradiation, the similar ferric oxide nanoparticles loaded with MFI zeolite could generate and stabilize N -oxyl radical formation, facilitating hydrocarbon oxidation into the corresponding ketones/carboxylic acids . Among other examples, analogous zeolite-mediated photocatalysts were used to treat volatile organic compounds (VOC), , degradation of organics diluted in water and air, photocatalytic reduction of CO 2 , and other relevant environmental applications. , …”

Section: Radical Chemistry In Zeolite Catalysismentioning

confidence: 99%

First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis

Gong

Çağlayan

et al. 2022

Chem. Rev.

View full text Add to dashboard Cite

Zeolite chemistry and catalysis are expected to play a decisive role in the next decade(s) to build a more decentralized renewable feedstock-dependent sustainable society owing to the increased scrutiny over carbon emissions. Therefore, the lack of fundamental and mechanistic understanding of these processes is a critical “technical bottleneck” that must be eliminated to maximize economic value and minimize waste. We have identified, considering this objective, that the chemistry related to the first-generation reaction intermediates (i.e., carbocations, radicals, carbenes, ketenes, and carbanions) in zeolite chemistry and catalysis is highly underdeveloped or undervalued compared to other catalysis streams (e.g., homogeneous catalysis). This limitation can often be attributed to the technological restrictions to detect such “short-lived and highly reactive” intermediates at the interface (gas–solid/solid–liquid); however, the recent rise of sophisticated spectroscopic/analytical techniques (including under in situ/operando conditions) and modern data analysis methods collectively compete to unravel the impact of these organic intermediates. This comprehensive review summarizes the state-of-the-art first-generation organic reaction intermediates in zeolite chemistry and catalysis and evaluates their existing challenges and future prospects, to contribute significantly to the “circular carbon economy” initiatives.

show abstract

Section: Radical Chemistry In Zeolite Catalysismentioning

confidence: 99%

First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis

Gong

Çağlayan

et al. 2022

Chem. Rev.

View full text Add to dashboard Cite

show abstract

“…On the other hand, natural minerals have high adsorption capacity, high thermochemical stability, low cost, convenient recycling, and rich content, which are good choices for the construction of macrosystems, such as kaolinite, [20] montmorillonite, [21] or zeolite. [22,23] Among them, vermiculite is a phyllosilicate mineral montmorillonite similar, which means a layer of the tetrahedral and octahedral ratio of 2 : 1 arrangement of composition, a thickness of about 1 nm or so, between the cell layer 2 is a layer of water molecules. Vermiculite has good cation exchange and adsorption properties, so it has a good application prospect in removing pollutants and the adsorption of heavy metal ions.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of CdS/g‐C₃N₄/Vermiculite Heterostructures with Enhanced Visible Photocatalytic Activity for Dye Degradation

Xue

Wang

et al. 2021

ChemistrySelect

View full text Add to dashboard Cite

In this study, CdS/g-C 3 N 4 /Vermiculite composites were prepared by hydrothermal and calcinated with expanded-vermiculite as host photocatalysis. Compared with other reference samples, the received CS/CN/VMT composite material has significantly enhanced photocatalytic activity on rhodamine B and methylene blue. The significantly enhanced catalytic efficiency is a benefit originating from the large specific surface area of vermiculite and the excellent electron transport efficiency between g-C 3 N 4 and CdS. Moreover, the degradation rate of the catalyst can still reach 96 % after being repeated four times, indicating that the composite catalyst has facilitated stability and recyclability. Particle capture experiments and ESR studies show that the * O 2 À is the primary active substance of CS/CN/VMT, and a possible photocatalytic degradation path has been proposed.

show abstract

“…Addition of butylated hydroxytoluene (BHT) completely suppressed the oxidation (Table , entry 12). The in situ electron paramagnetic resonance (EPR) clearly demonstrated the formation of PINO radical in accordance with previous reports , (Figure a). Conversely, no PINO signal was observed, even with the good peroxide decomposition catalyst such as Ru(acac) 3 , indicating PINO generation boosted by bisCu (Figure b).…”

mentioning

confidence: 99%

“…The Xu group used anthraquinone derivatives as the biomimetic SET reagent to accelerate the PINO-mediated oxidation of ethylbenzene . Notably, Xiao and Wang have both reported the innovative methods to achieve ambient oxidation of benzylic and cyclic C–H bonds, via stabilizing the photogenerated PINO radicals inside the FeO x /zeolite and on the surface of α-Fe 2 O 3 , respectively.…”

mentioning

confidence: 99%

Selective Functionalization of Hydrocarbons Using a ppm Bioinspired Molecular Tweezer via Proton-Coupled Electron Transfer

Chen

Wang

et al. 2021

ACS Catal.

View full text Add to dashboard Cite

An expanded porphyrin-biscopper hexaphyrin was introduced as a bioinspired molecular tweezer to co-catalyze functionalization of C(sp3)–H bonds. Theoretical and experimental investigations suggested that the biscopper hexaphyrin served as a molecular tweezer to mimic the enzymatic orientation/proximity effect, efficiently activating the N-hydroxyphthalimide (NHPI) via light-free proton-coupled electron transfer (PCET), at an exceptionally low catalyst loading of 10 mol ppm. The resulting N-oxyl radical (PINO) was versatile for chemoselective C–H oxidation and amination of hydrocarbons.

show abstract

N-Oxyl Radicals Trapped on Zeolite Surface Accelerate Photocatalysis

Cited by 18 publications

References 35 publications

First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis

First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis

Synthesis of CdS/g‐C₃N₄/Vermiculite Heterostructures with Enhanced Visible Photocatalytic Activity for Dye Degradation

Selective Functionalization of Hydrocarbons Using a ppm Bioinspired Molecular Tweezer via Proton-Coupled Electron Transfer

Contact Info

Product

Resources

About

N-Oxyl Radicals Trapped on Zeolite Surface Accelerate Photocatalysis

Cited by 18 publications

References 35 publications

First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis

First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis

Synthesis of CdS/g‐C3N4/Vermiculite Heterostructures with Enhanced Visible Photocatalytic Activity for Dye Degradation

Selective Functionalization of Hydrocarbons Using a ppm Bioinspired Molecular Tweezer via Proton-Coupled Electron Transfer

Contact Info

Product

Resources

About

Synthesis of CdS/g‐C₃N₄/Vermiculite Heterostructures with Enhanced Visible Photocatalytic Activity for Dye Degradation