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[摘要]：Photoelectrochemical cells based on traditional and nanostructured ZnO thin films are investigated for hydrogen generation from water splitting. The ZnO thin films are fabricated using three different deposition geometries: normal pulsed laser deposition, pulsed laser oblique-angle deposition, and electron-beam glancing-angle deposition. The nanostructured films are characterized by scanning electron microscopy, X-ray diffraction, UV-vis spectroscopy and photoelectrochemical techniques. Normal pulsed laser deposition produces dense thin films with ca. 200 nm grain sizes, while oblique-angle deposition produces nanoplatelets with a fishscale morphology and individual features measuring ca. 900 by 450 nm on average. In contrast, glancing-angle deposition generates a highly porous, interconnected network of spherical nanoparticles of 15-40 nm diameter. Mott-Schottky plots show the flat band potential of pulsed laser deposition, oblique-angle deposition, and glancing-angle deposition samples to be -0.29, -0.28 and +0.20V, respectively. Generation of photocurrent is observed at anodic potentials and no limiting photocurrents; were observed with applied potentials up to 1.3 V for all photoelectrochemical cells. The effective photon-to-hydrogen efficiency is found to be 0.1%, 0.2% and 0.6% for pulsed laser deposition, oblique-angle deposition and glancing-angle deposition samples, respectively. The photoelectrochemical properties of the three types of films are understood to be a function of porosity, crystal defect concentration, charge transport properties and space charge layer characteristics. |
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