Dinitrogen Fixation Using Conducting Polymer/Titanium Oxide Junction

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Nitrogen fixation systems driven by white light under mild conditions was investigated. The typical system consists of titanium oxide (TiO_x) and poly(3-methylthiophene)(P3MeT), and their heterojunction is previously shown to produce ammonium salt crystals (NH_4ClO_4) when exposed to white light in air at 20℃ and 40%RH. The purpose of this study is to identify the nitrogen-fixation products and to obtain the information on the fixation mechanism. X-ray photoelectron spectroscopic analyzes of the junctions before and after the photoirradiation revealed that ammonia is also formed as one of the fixation products. Additionaly, the combination of quantification of the products and electron-dispersive analysis of X-rays revealed that the reaction is initiated by annmonia formation (at the TiO_x/P3MeT interface) and followed by its partial conversion into NH_4ClO_4 in the P3MeT bulk. Further investigations showed the contribution of water molecules and polaron/biporaron species in the P3MeT film to the fixation reaction. These results led to the materials/device structures and increasing the efficiency of the light-to-chemical energy conversion.