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Bifunctionality of dirhodium tetracarboxylates in metallaphotocatalysis

Author

Listed:
  • Taoda Shi

    (Sun Yat-sen University)

  • Tianyuan Zhang

    (Sun Yat-sen University)

  • Jiying Yang

    (Sun Yat-sen University)

  • Yukai Li

    (Sun Yat-sen University)

  • Jirong Shu

    (Sun Yat-sen University)

  • Jingyu Zhao

    (Sun Yat-sen University)

  • Mengchu Zhang

    (Sun Yat-sen University)

  • Dan Zhang

    (Sun Yat-sen University)

  • Wenhao Hu

    (Sun Yat-sen University)

Abstract

Metallaphotocatalysis has been recognized as a pivotal catalysis enabling new reactivities. Traditional metallaphotocatalysis often requires two or more separate catalysts and exhibits flaw in cost and substrate-tolerance, thus representing an await-to-solve issue in catalysis. We herein realize metallaphotocatalysis with a bifunctional dirhodium tetracarboxylate ([Rh2]) alone. The [Rh2] shows an photocatalytic activity of promoting singlet oxygen (1O2) oxidation. By harnessing its photocatalytic activity, the [Rh2] catalyzes a photochemical cascade reaction (PCR) via combination of carbenoid chemistry and 1O2 chemistry. The PCR is characterized by high atom-efficiency, excellent stereoselectivities, mild conditions, scalable synthesis, and pharmaceutically interesting products. DFT calculations-aided mechanistic study rationalizes the reaction pathway and interprets the origin of stereoselectivities of the PCR. The products show inhibitory activity against PTP1B, being promising in the treatment of type II diabetes and cancers. Overall, here we show the bifunctional [Rh2] merges Rh-carbenoid chemistry and 1O2 chemistry.

Suggested Citation

  • Taoda Shi & Tianyuan Zhang & Jiying Yang & Yukai Li & Jirong Shu & Jingyu Zhao & Mengchu Zhang & Dan Zhang & Wenhao Hu, 2023. "Bifunctionality of dirhodium tetracarboxylates in metallaphotocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43050-3
    DOI: 10.1038/s41467-023-43050-3
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    References listed on IDEAS

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    1. Sifan Yu & Wenju Chang & Ruyu Hua & Xiaoting Jie & Mengchu Zhang & Wenxuan Zhao & Jinzhou Chen & Dan Zhang & Huang Qiu & Yong Liang & Wenhao Hu, 2022. "An enantioselective four-component reaction via assembling two reaction intermediates," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Liuzhuang Xing & Qian Yang & Chen Zhu & Yilian Bai & Yurong Tang & Magnus Rueping & Yunfei Cai, 2023. "Poly(heptazine imide) ligand exchange enables remarkable low catalyst loadings in heterogeneous metallaphotocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Kuangbiao Liao & Solymar Negretti & Djamaladdin G. Musaev & John Bacsa & Huw M. L. Davies, 2016. "Site-selective and stereoselective functionalization of unactivated C–H bonds," Nature, Nature, vol. 533(7602), pages 230-234, May.
    4. Haohua Huo & Xiaodong Shen & Chuanyong Wang & Lilu Zhang & Philipp Röse & Liang-An Chen & Klaus Harms & Michael Marsch & Gerhard Hilt & Eric Meggers, 2014. "Asymmetric photoredox transition-metal catalysis activated by visible light," Nature, Nature, vol. 515(7525), pages 100-103, November.
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