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Hybridisation is a powerful strategy towards the next generation ofmultifunctional materials for environmental and sustainable energyapplications. Here, we report a new inorganic nanocarbon hybrid materialprepared with atomically controlled deposition of a monocrystalline TiO2 layerthat conformally coats a macroscopic carbon nanotube (CNT) fiber. Through X-raydiffraction, Raman spectroscopy and photoemission spectroscopy we detect theformation of a covalent Ti-O-C bond at the TiO2/CNT interface and a residualstrain of approximately 0.7-2 \%, which is tensile in TiO2 and compressive inthe CNT. It arises after deposition of the amorphous oxide onto the CNT surfacepreviously functionalized by the oxygen plasma used in ALD. These features areobserved in samples of different TiO2 thickness, in the range from 10 to 80 nm.Ultraviolet photoemission spectroscopy on a 20 nm-thick TiO2 coated samplegives a work function of 4.27 eV, between that of TiO2 (4.23 eV) and the CNTfiber (4.41 eV), and the presence of new interband gap states that shift thevalence band maximum to 1.05 eV below the Fermi level. Photoelectrochemicalmeasurements demonstrate electron transfer from TiO2 to the CNT fiber networkunder UV irradiation. Electrochemical impedance spectroscopy measurementsreveal a low resistance for charge transfer and transport, as well as a largecapacitance. Our results point to the fact that these hybrids, in which eachphase has nanometric thickness and the current collector is integrated into thematerial, are very different from conventional electrodes and can provide anumber of superior properties.

Large area photoelectrodes based on hybrids of CNT fibres and ALD grown TiO2