Inside Cover: A Cooperative Rhodium/Secondary Phosphine Oxide [Rh/P(O)<i>n</i>Bu<sub>2</sub>] Template for Catalytic Hydrodefluorination of Perfluoroarenes (Angew. Chem. Int. Ed. 23/2023)

Chang, Wei-Chieh; Randel, Helena; Weyhermüller, Thomas; Auer, Alexander A.; Farès, Christophe; Werlé, Christophe

doi:10.1002/anie.202303992

Angew Chem Int Ed

2023

DOI: 10.1002/anie.202303992

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Inside Cover: A Cooperative Rhodium/Secondary Phosphine Oxide [Rh/P(O)nBu₂] Template for Catalytic Hydrodefluorination of Perfluoroarenes (Angew. Chem. Int. Ed. 23/2023)

Wei-Chieh Chang

Helena Randel

Thomas Weyhermüller

et al.

Abstract: Twoc ooperative arms ……[ Rh/P(O)nBu 2 ]a re in the process of activating and breaking CÀFb onds to create CÀHbonds.Intheir Research Article (e202219127), Christophe WerlØ and co-workers developed amolecular template based on these design elements to improve the catalytic hydrodefluorination of perfluoroarenes across aw ide range of substrates.

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“…The focal point of our research program encompasses the advancement of dynamic and adaptive molecular systems capable of facilitating complex bond activations . Such systems are particularly salient in the domain of chemical energy conversion, where obstacles arise due to variable energy supplies and inconsistent feedstock quality.…”

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confidence: 99%

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (Z)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity

Jena,

Frenzen,

Chugh

et al. 2023

J. Am. Chem. Soc.

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confidence: 99%

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (Z)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity

Jena,

Frenzen,

Chugh

et al. 2023

J. Am. Chem. Soc.

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Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh–Pd/C Catalysts

Gong,

Qin,

et al. 2024

ACS Appl. Mater. Interfaces

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This study explores the synergistic effect between the Rh and Pd of bimetallic Rh–Pd/C catalysts for the catalytic hydro-defluorination (HDF) of 4-fluorophenol (4-FP). It was found that 4-FP could not be efficiently hydro-defluorinated over 6% Pd/C and 6% Rh/C due to the inherent properties of Pd and Rh species in the dissociation of H2 and the activation of C–F bonds. Compared with 6% Pd/C and 6% Rh/C, bimetallic Rh–Pd/C catalysts, especially 1% Rh–5% Pd/C, exhibited much higher catalytic activity in the HDF of 4-FP, suggesting that the synergistic effect between the Rh and Pd of the catalyst was much more positive. Catalyst characterizations (BET, XRD, TEM, and XPS) were introduced to clarify the mechanism for the synergistic effect between the Rh and Pd of the catalyst in the HDF reaction and revealed that it was mainly attributed to the bifunctional mechanism: Pd species were favorable for the dissociation of H2, and Rh species were beneficial to the activation of C–F bonds in the HDF reaction. Meanwhile, the interaction between Rh and Pd species enabled Rh and Pd to exhibit a more positive synergistic effect, which promoted the migration of atomic H* from Pd to Rh species and thus enhanced the HDF of 4-FP. Furthermore, 1% Rh–5% Pd/C prepared using 20–40 equiv NaBH4 exhibited the best performance in the catalytic HDF of 4-FP. Catalysis characterizations suggested that appropriate Rh3+/Rh0 and Pd2+/Pd0 ratios were beneficial to the dissociation of H2 and the activation of C–F bonds, which caused the more positive synergistic effect between the Rh and Pd of Rh–Pd/C in the HDF reaction. This work offers a valuable strategy for enhancing the performance of catalytic HDF catalysts via promoting synergistic effects.

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Inside Cover: A Cooperative Rhodium/Secondary Phosphine Oxide [Rh/P(O)nBu₂] Template for Catalytic Hydrodefluorination of Perfluoroarenes (Angew. Chem. Int. Ed. 23/2023)

Cited by 2 publications

References 0 publications

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (Z)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (Z)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity

Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh–Pd/C Catalysts

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Inside Cover: A Cooperative Rhodium/Secondary Phosphine Oxide [Rh/P(O)nBu2] Template for Catalytic Hydrodefluorination of Perfluoroarenes (Angew. Chem. Int. Ed. 23/2023)

Cited by 2 publications

References 0 publications

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (Z)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (Z)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity

Novel Insight into the Synergistic Mechanism for Pd and Rh Promoting the Hydro-Defluorination of 4-Fluorophenol over Bimetallic Rh–Pd/C Catalysts

Contact Info

Product

Resources

About

Inside Cover: A Cooperative Rhodium/Secondary Phosphine Oxide [Rh/P(O)nBu₂] Template for Catalytic Hydrodefluorination of Perfluoroarenes (Angew. Chem. Int. Ed. 23/2023)