Single-walled carbon nanotubes (SWNTs) are expected to be a promising nanomaterial because of their outstanding electronic, mechanical, and thermal properties. For macroscopic device applications, an assembly of SWNTs is a critical issue. We propose a self-organized micro-honeycomb network structure of SWNTs obtained by water vapor treatment of as-synthesized vertically-aligned SWNTs (VA-SWNT) for solar cell devices with higher performance. The micro-honeycomb structure was realized by simply exposing VA-SWNT to water vapor and drying in ambient condition. Honeycomb cell walls consist of capillary-aggregated vertically aligned SWNTs with heavily bundled top part. Within each cell, collapsed spaghetti-like SWNTs make contact to the substrate. The SWNT/n-Si heterojunction solar cell was built by placing the micro-honeycomb SWNTs network film on top of the substrate which has a 3 mm × 3 mm bare n-type silicon contact window in the center. The contact window is surrounded by SiO2 as insulating layer and Pt as electrode. Our preliminary tests showed that optimal photovoltaic conversion efficiency (PCE) under AM1.5 was 5.91%, with the fill factor of 72%. The open-circuit voltage and short-circuit current are 0.53V and 15.5 mA/cm2, respectively. This showed a substantial improvement compared with heterojunction solar cells using spaghetti-like SWNTs. Furthermore, the superior performance of dye-sensitized solar cells with the micro-honeycomb SWNTs was demonstrated.

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