室温作動の安価なプロトン導電性固体電解質の開発

本研究的目的是寻找在200-300℃中温下工作的无机质子导体。制备并测试以下三种类型的材料。(1)采用醇盐水解法制备了吸水陶瓷颗粒。在这样的低温合成中，颗粒不能很好地生长并且表面积变得相当大。合成的陶瓷有TiO_2，Al_2O_3，ZrO_2，SiO_2，BaTiO_3。在90℃下测得的电导率落在10 <-4>- 10 μ <-3>Scm 2之间<-1>。在相同温度下，在温度升高和降低的方向上测量的电导率不一致。后者总是比前者小。质子可以通过吸附的水分子传导，并且受其量的显著影响。因此，它显示了对温度曲线的滞后。(2)为了通过吸附的水分子增加电导率，提高质子浓度。通过在ZrO_2颗粒表面固载SO_4 ~（2-）官能团制备了超强酸<2->。但与纯ZrO_2相比，电导率只有很小的提高。(3)本文选择了新型的Ln（OH）_3（Ln：La_（3+））材料作为研究对象。Ln（OH）_3的电导率随稀土元素的变化范围较宽，且在加热和冷却循环过程中具有较小的滞后现象。电导率为10 μ m <-2>× 10 μ m <-3>× 10 μ m<-1>。这些材料仍有待讨论，但有可能质子主要通过OH键之间的跳跃移动。

The objective of the study is to search for inorganic proton conductors operating at medium temperatures as 200-300℃. Three types of materials below were prepared and tested.(1) Water adsorbed ceramic particles were prepared by hydrolysis of alkoxide. In such a low-temperature synthesis, particle does not grow well and surface area becomes fairly large. The synthesized ceramics are TiO_2, A1_2O_3, ZrO_2, SiO_2, BaTiO_3. The conductivities measured at 90℃ fall into the range between 10^<-4> and 10^<-3>Scm^<-1>. The conductivities measured in the directions of temperature increase and decrease do not coincide at the same temperature. The latter is always smaller than the former. Protons may conduct via adsorbed water molecules and be significantly affected by their amount. Thus, it shows the hysteresis against temperature profile.(2) To increase the conductivity via adsorbed water molecules, protonic concentration was enhanced. Super strong acid was prepared by fixing SO_4^<2-> functional group on the surface of ZrO_2 particles. However, only small improvement of the conductivity in comparison to pure ZrO_2 particle was observed.(3) Novel Ln(OH)_3(Ln : Lanthanide) materials were chosen for investigation. Ln(OH)_3 showed wide range of conductivities depending on lanthanide element and less hysteresis during heating and cooling cycle. The conductivities are 10^<-2>〜10^<-3>Scm^<-1>. These materials still open for discussion, but have possibility that proton move mainly by hopping between OH bonds.