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Site Isolation in Metal–Organic Layers Enhances Photoredox Gold Catalysis

https://doi.org/10.1021/jacs.2c03062

Zheng, Haifeng ; Fan, Yingjie ; Song, Yang ; Chen, Justin S. ; You, Eric ; Labalme, Steven ; Lin, Wenbin ( June 2022 , Journal of the American Chemical Society)

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A Substrate-Binding Metal–Organic Layer Selectively Catalyzes Photoredox Ene-Carbonyl Reductive Coupling Reactions

https://doi.org/10.1021/jacs.1c10180

Fan, Yingjie ; You, Eric ; Xu, Ziwan ; Lin, Wenbin ( November 2021 , Journal of the American Chemical Society)

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Metal–Organic Layers Hierarchically Integrate Three Synergistic Active Sites for Tandem Catalysis

https://doi.org/10.1002/anie.202011519

Quan, Yangjian ; Lan, Guangxu ; Shi, Wenjie ; Xu, Ziwan ; Fan, Yingjie ; You, Eric ; Jiang, Xiaomin ; Wang, Cheng ; Lin, Wenbin ( December 2020 , Angewandte Chemie International Edition)

Abstract
We report the design of a bifunctional metal–organic layer (MOL), Hf₁₂‐Ru‐Co, composed of [Ru(DBB)(bpy)₂]²⁺[DBB‐Ru, DBB=4,4′‐di(4‐benzoato)‐2,2′‐bipyridine; bpy=2,2′‐bipyridine] connecting ligand as a photosensitizer and Co(dmgH)₂(PPA)Cl (PPA‐Co, dmgH=dimethylglyoxime; PPA=4‐pyridinepropionic acid) on the Hf₁₂secondary building unit (SBU) as a hydrogen‐transfer catalyst. Hf₁₂‐Ru‐Co efficiently catalyzed acceptorless dehydrogenation of indolines and tetrahydroquinolines to afford indoles and quinolones. We extended this strategy to prepare Hf₁₂‐Ru‐Co‐OTf MOL with a [Ru(DBB)(bpy)₂]²⁺photosensitizer and Hf₁₂SBU capped with triflate as strong Lewis acids and PPA‐Co as a hydrogen transfer catalyst. With three synergistic active sites, Hf₁₂‐Ru‐Co‐OTf competently catalyzed dehydrogenative tandem transformations of indolines with alkenes or aldehydes to afford 3‐alkylindoles and bisindolylmethanes with turnover numbers of up to 500 and 460, respectively, illustrating the potential use of MOLs in constructing novel multifunctional heterogeneous catalysts.

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Metal–Organic Layers Hierarchically Integrate Three Synergistic Active Sites for Tandem Catalysis

https://doi.org/10.1002/ange.202011519

Quan, Yangjian ; Lan, Guangxu ; Shi, Wenjie ; Xu, Ziwan ; Fan, Yingjie ; You, Eric ; Jiang, Xiaomin ; Wang, Cheng ; Lin, Wenbin ( December 2020 , Angewandte Chemie)

Abstract
We report the design of a bifunctional metal–organic layer (MOL), Hf₁₂‐Ru‐Co, composed of [Ru(DBB)(bpy)₂]²⁺[DBB‐Ru, DBB=4,4′‐di(4‐benzoato)‐2,2′‐bipyridine; bpy=2,2′‐bipyridine] connecting ligand as a photosensitizer and Co(dmgH)₂(PPA)Cl (PPA‐Co, dmgH=dimethylglyoxime; PPA=4‐pyridinepropionic acid) on the Hf₁₂secondary building unit (SBU) as a hydrogen‐transfer catalyst. Hf₁₂‐Ru‐Co efficiently catalyzed acceptorless dehydrogenation of indolines and tetrahydroquinolines to afford indoles and quinolones. We extended this strategy to prepare Hf₁₂‐Ru‐Co‐OTf MOL with a [Ru(DBB)(bpy)₂]²⁺photosensitizer and Hf₁₂SBU capped with triflate as strong Lewis acids and PPA‐Co as a hydrogen transfer catalyst. With three synergistic active sites, Hf₁₂‐Ru‐Co‐OTf competently catalyzed dehydrogenative tandem transformations of indolines with alkenes or aldehydes to afford 3‐alkylindoles and bisindolylmethanes with turnover numbers of up to 500 and 460, respectively, illustrating the potential use of MOLs in constructing novel multifunctional heterogeneous catalysts.

more » « less