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A metal-organic cage incorporating multiple light harvesting and catalytic centres for photochemical hydrogen production

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  • Sha Chen

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Kang Li

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Fang Zhao

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Lei Zhang

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Mei Pan

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Yan-Zhong Fan

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Jing Guo

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Jianying Shi

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University)

  • Cheng-Yong Su

    (MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University
    State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences)

Abstract

Photocatalytic water splitting is a natural but challenging chemical way of harnessing renewable solar power to generate clean hydrogen energy. Here we report a potential hydrogen-evolving photochemical molecular device based on a self-assembled ruthenium–palladium heterometallic coordination cage, incorporating multiple photo- and catalytic metal centres. The photophysical properties are investigated by absorption/emission spectroscopy, electrochemical measurements and preliminary DFT calculations and the stepwise electron transfer processes from ruthenium-photocentres to catalytic palladium-centres is probed by ultrafast transient absorption spectroscopy. The photocatalytic hydrogen production assessments reveal an initial reaction rate of 380 μmol h−1 and a turnover number of 635 after 48 h. The efficient hydrogen production may derive from the directional electron transfers through multiple channels owing to proper organization of the photo- and catalytic multi-units within the octahedral cage, which may open a new door to design photochemical molecular devices with well-organized metallosupramolecules for homogenous photocatalytic applications.

Suggested Citation

  • Sha Chen & Kang Li & Fang Zhao & Lei Zhang & Mei Pan & Yan-Zhong Fan & Jing Guo & Jianying Shi & Cheng-Yong Su, 2016. "A metal-organic cage incorporating multiple light harvesting and catalytic centres for photochemical hydrogen production," Nature Communications, Nature, vol. 7(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13169
    DOI: 10.1038/ncomms13169
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    Cited by:

    1. Yingguo Li & Jialun He & Guilong Lu & Chensheng Wang & Mengmeng Fu & Juan Deng & Fu Yang & Danfeng Jiang & Xiao Chen & Ziyi Yu & Yan Liu & Chao Yu & Yong Cui, 2024. "De novo construction of amine-functionalized metal-organic cages as heterogenous catalysts for microflow catalysis," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Jin Ming Wang & Qin Yao Zhu & Jeong Heon Lee & Tae Gyun Woo & Yue Xing Zhang & Woo-Dong Jang & Tae Kyu Kim, 2023. "Asymmetric gradient orbital interaction of hetero-diatomic active sites for promoting C − C coupling," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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