A highly dispersible and stable nanocomposite of Cu(tpa)-GO (Cu(tpa) = copper terephthalate metal-organic framework, GO = graphene oxide) was prepared through a simple ultrasonication method. The morphology and structure of the obtained composite were characterized via scanning electron microscopy (SEM), transmission electron microscopy (TEM), UV-vis, Fourier-transform infrared (FT-IR), X-ray diffraction (XRD), and thermogravimetric analysis (TGA). On the basis of the characterization results, the binding mechanism of the Cu(tpa) and GO was speculated to be the cooperative interaction of π-π stacking, hydrogen bonding, and Cu-O coordination. The electrochemical sensing property of Cu(tpa)-GO composite was investigated through casting the composite on a glassy carbon electrode (GCE), followed by an electro-reduction treatment to transfer the GO in the composite to the highly conductive reduced form (electrochemically reduced graphene, EGR). The results demonstrated that the electrochemical signals and peak profiles of the two drugs of acetaminophen (ACOP) and dopamine (DA) were significantly improved by the modified material, owing to the synergistic effect from high conductivity of EGR and unique electron mediating action of Cu(tpa). Under the optimum conditions, the oxidation peak currents of ACOP and DA were linearly correlated to their concentrations in the ranges of 1-100 and 1-50 μM, respectively. The detection limits for ACOP and DA were estimated to be as low as 0.36 and 0.21 μM, respectively.
A synthetic five-part molecular device has been prepared that uses a multistep electron transfer strategy similar to that of photosynthetic organisms to capture light energy and convert it to chemical potential in the form of long-lived charge separation. It consists of two covalently linked porphyrin moieties, one containing a zinc ion (P(Zn)) and the other present as the free base (P). The metailated porphyrin bears a carotenoid polyene (C) and the other a diquinone species (Q(A)-Q(B)). Excitation of the free-base porphyrin in a chloroform solution of the pentad yields an initial charge-separated state, C-P(Zn)-P(.+).-Q(A)(-)-Q(B), with a quantum yield of 0.85. Subsequent electron transfer steps lead to a final charge-separated state, C(.+)-P(Zn)-P-Q(A)-Q(B)(.-), which is formed with an overall quantum yield of 0.83 and has a lifetime of 55 microseconds. Irradiation of the free-base form of the pentad, C-P-P-Q(A)-Q(B), gives a similar charge-separated state with a lower quantum yield (0.15 in dichloromethane), although the lifetime is increased to approximately 340 microseconds. The artificial photosynthetic system preserves a significant fraction ( approximately 1.0 electron volt) of the initial excitation energy (1.9 electron volts) in the long-lived, charge-separated state.
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