(Terpyridine)copper(II)−Carbon Nanohorns:  Metallo-nanocomplexes for Photoinduced Charge Separation

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  • Georgios Rotas
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan
  • Atula S. D. Sandanayaka
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan
  • Nikos Tagmatarchis
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan
  • Toshinari Ichihashi
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan
  • Masako Yudasaka
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan
  • Sumio Iijima
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan
  • Osamu Ito
    Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vass. Constantinou Ave., Athens 116 35, Greece, Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Aoba-ku, Sendai 980-8577, Japan, and SORST, Japan Science and Technology Agency, NEC Corporation, 34 Miyukigaoka, Tsukuba, Ibaraki 305-8501, Japan

説明

New metallo-nanostructured materials of carbon nanohorns (CNHs), within the family of elongated carbon nanotubes, have been prepared by the coordination of copper(II)-2,2':6',2' '-terpyridine (Cu(II)tpy) with oxidized carbon nanohorns (CNHs-COOH). The resulted CNHs-COO-Cu(II)tpy metallo-nanocomplexes have been characterized by diverse analytical spectroscopic tools and cyclic and differential pulse voltammetry. Scanning transmission electron microscopy (STEM), dynamic light scattering (DLS), and energy dispersive X-ray spectroscopy (EDX) measurements have been employed to probe the morphological characteristics and particle-size distribution of CNHs-COO-Cu(II)tpy as well as to investigate the elemental composition of the metallo-nanocomplex. Steady-state and time-resolved fluorescence emission studies have shown efficient fluorescence quenching, suggesting that electron transfer occurs from the singlet excited state of Cu(II)tpy to CNHs. Photoexcitation of Cu(II)tpy resulted in the one-electron reduction of nanohorns with a simultaneous one-electron oxidation of the Cu(II)tpy unit (CNHs(*-)-COO-(Cu(II)tpy)*+) as revealed by transient absorption measurements. The charge-separated state of CNHs(*-)-COO-(Cu(II)tpy)*+ has been confirmed with the aid of an electron mediator, such as hexyl-viologen dication (HV2+) and an electron-hole shifter in polar solvents.

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