Photoinduction of palladium single atoms supported on defect-containing γ-AlOOH nanoleaf for efficient trans-stilbene epoxidation

Li, Zhijun; Li, Honghong; Yuan, Dundong; Leng, Leipeng; Zhang, Mingyang; Di, Minghui; Horton, J. Hugh; Wang, Jun; Sun, Litao; Sun, Weiwei

doi:10.1016/j.cej.2021.132149

Cited by 8 publications

(4 citation statements)

References 56 publications

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“…[12] As a new frontier, single atom catalysts (SACs) have gained wide attention because of their great advantages of high atom efficiency and unique catalytic activity. [13][14][15][16][17][18][19][20] SACs possess distinctive chemical and physical properties and a unique coordination environment that is different from their nanoparticle counterparts. [21][22][23][24][25] Moreover, SACs have been found to be effective in bridging homogeneous and heterogeneous catalysis.…”

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confidence: 99%

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Fan

et al. 2022

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Lee et al. reported a series of highly active single-site mesoporous Pd/Al 2 O 3 catalysts for selective aerobic oxidation of allylic alcohols. [9] Grassi et al. described gold nanoparticles enclosed in a polymer matrix for oxidative esterification of cinnamyl alcohol with alkyl alcohols. [10] Lee and co-workers developed a zirconia-supported ruthenium catalyst for efficient aerobic oxidation of alcohols to aldehydes. [11] Li et al. found that metal/oxide supported catalysts, such as FeO/Pt(111) or Cu 2 O/ Ag(111) exhibit interfacial effects that significantly improve the efficacy in the selective oxidation of primary alcohols. [4] These nanoparticle-based catalysts, though effective in mediating selective oxidation reactions, have significant drawbacks of high cost, low selectivity, and rapid deactivation in harsh conditions. As such, the development of more practical and economical catalyst systems has been a major challenge in both industrial and academic areas.In 2011, Zhang and co-workers, for the first time, presented a comprehensive study and coined the concept of single-atom catalysis. [12] As a new frontier, single atom catalysts (SACs) have gained wide attention because of their great advantages of high atom efficiency and unique catalytic activity. [13][14][15][16][17][18][19][20] SACs possess distinctive chemical and physical properties and a unique coordination environment that is different from their nanoparticle counterparts. [21][22][23][24][25] Moreover, SACs have been found to be effective in bridging homogeneous and heterogeneous catalysis. [26][27][28][29] Selective aerobic oxidation of alcohols offers an attractive means to address challenges in the modern chemical industry, but the development of nonnoble metal catalysts with superior efficacy for this reaction remains a grand challenge. Here, this study reports on such a catalyst based on atomically defined undercoordinated copper atoms over nitrogen-doped carbon support as an efficient, durable, and scalable heterogeneous catalyst for selective aerobic oxidation of alcohols. This catalyst exhibits extremely high intrinsic catalytic activity (TOF of 7692 h −1 ) in the oxidation of cinnamyl alcohol to afford cinnamaldehyde, along with exceptional recyclability (at least eight cycles), scalability, and broad substrate scope. DFT calculations suggest that the high activity derives from the low oxidation state and the unique co ordination environment of the copper sites in the catalyst. These findings pave the way for the design of highly active and stable single atom catalysts to potentially address challenges in synthetic chemistry.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202106614.

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Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Fan

et al. 2022

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“…Furthermore, X-ray absorption spectroscopy (XAS) studies were performed to provide further evidence for the local structure of Pd species on FeO x . The Fourier transform (FT) radial distribution functions of the k 3 -weight extended X-ray absorption fine structure (EXAFS) spectrum (Figure 2b) for Pd 1 /FeO x -10 at the Pd K edge showed that an obvious peak at ∼1.5 Å was ascribed to the Pd−O bond in comparison with the reference samples of Pd foil and PdO, strongly suggesting atomic dispersion of Pd atoms, 14 in agreement with the AC HAADF-STEM results. To obtain the coordination information of Pt atoms, EXAFS fitting was also carried out (Figure S2 and Table S2).…”

Section: Resultsmentioning

confidence: 99%

Highly Efficient Fabrication of Kilogram-Scale Palladium Single-Atom Catalysts for the Suzuki–Miyaura Cross-Coupling Reaction

Zhang

Shi

et al. 2022

ACS Appl. Mater. Interfaces

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Palladium single-atom catalysts (SACs) have caught great attention owing to their maximal atom utilization and outstanding activity for the Suzuki–Miyaura cross-coupling reaction. However, a facile manufacturing method for kilogram-scale synthesis of noble metal SACs with high productivity is still in demand. This study reports on the synthesis of SACs by direct ball milling of commercial metal oxides and nitrate precursors with a productivity of ∼100%. The as-prepared Pd1/FeO x SACs show high catalytic performance (the TOFs are 7844 h–1), high stability, and general applicability for the Suzuki–Miyaura cross-coupling reaction under mild conditions. More encouragingly, kilogram-scale Pd1/FeO x SACs can be synthesized in one batch by this approach, endowing great potential for industrial applications. Furthermore, the preparation of Pt, Ru, and Rh SACs is also successfully carried out via the ball milling method, demonstrating favorable applicability. Our findings illustrate exciting chances presented by the highly efficient synthesis of SACs for the formation of C–C bonds.

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“…The Co-N x active site showed high intrinsic activity in the epoxidation of cyclooctene at 140 • C, and the yield of the target product (1,2-epoxycycloheptane) reached 95% [47]. Moreover, the oxide materials are also capable of introducing a large number of vacancies in SACs [48]. For example, Bi vacancies in Ru 1 /Bi 2−x WO 6 SACs can confine Ru species at an atomic scale and provide exceptional efficiency in the epoxidation of trans-stilbene to trans-stilbene oxide [49].…”

Section: Epoxidationmentioning

confidence: 99%

Recent Development of Single-Atom Catalysis for the Functionalization of Alkenes

Yan

et al. 2023

Catalysts

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The functionalization of alkenes is one of the most important conversions in synthetic chemistry to prepare numerous fine chemicals. Typical procedures, such as hydrosilylation and hydroformylation, are traditionally catalyzed using homogeneous noble metal complexes, while the highly reactive and stable heterogeneous single-atom catalysts (SACs) now provide alternative approaches to fulfill these conversions by combining the advantages of both homogeneous catalysts and heterogeneous nanoparticle catalysts. In this review, the recent achievement in single-atom catalyzed hydrosilylation and hydroformylation reactions are introduced, and we highlight the latest applications of SACs for additive reactions, constructing new C-Y (Y = B, P, S, N) bonds on the terminal carbon atoms of alkenes, and then mention the applications in single-metal-atom catalyzed hydrogenation and epoxidation reactions. We also note that some tandem reactions are conveniently realized in one pot by the concisely fabricated SACs, facilitating the preparation of some pharmaceutical compounds. Lastly, the challenges facing single-atom catalysis for alkene conversions are briefly mentioned.

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Photoinduction of palladium single atoms supported on defect-containing γ-AlOOH nanoleaf for efficient trans-stilbene epoxidation

Cited by 8 publications

References 56 publications

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Highly Efficient Fabrication of Kilogram-Scale Palladium Single-Atom Catalysts for the Suzuki–Miyaura Cross-Coupling Reaction

Recent Development of Single-Atom Catalysis for the Functionalization of Alkenes

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