In this study we report on the electrodeposition of copper thiocynate (CuSCN) nanorod arrays on ITO substrate from an EDTA-chelated aqueous solution. Effects of molecule ratio of EDTA/Cu²⁺ and deposition time on the properties of CuSCN layers were studied. Results showed that films deposited from an electrolyte with low EDTA amounts were consisted of densely packed nano-crystals, while films deposited with high molecule ratios of EDTA/Cu²⁺ (>0.5) were composed of homogeneous nanorods with their (001) plane perpendicular to the substrate. Further time-dependent study showed that the formation of CuSCN nanorods was initiated at the very beginning of potential application and no intermediate or transitional products were detected during the electrochemical process. Optical analysis showed that films of CuSCN nanorods with a thickness of 100–400 nm had good optical quality, and exhibited the fundamental absorption edge at 320 nm.
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