Synthesis of proton conductive inorganic–organic hybrid membranes from organoalkoxysilane and hydroxyalkylphosphonic acid

Synthesis of proton conductive inorganic–organic hybrid membranes from organoalkoxysilane and hydroxyalkylphosphonic acid
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DOI:
10.1016/j.memsci.2008.11.005
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发表时间:
2009-01
影响因子:
9.5
通讯作者:
Junji Umeda;M. Moriya;W. Sakamoto;T. Yogo
Junji Umeda;M. Moriya;W. Sakamoto;T. Yogo
中科院分区:
工程技术1区
文献类型:
--
作者:
Junji Umeda;M. Moriya;W. Sakamoto;T. Yogo

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以3-缩水甘油氧基丙基三甲氧基硅烷(GPTMS)、苯基三乙氧基硅烷(PhTES)和羟烷基膦酸为原料合成了质子导电无机-有机杂化膜。两种羟基烷基膦酸,1-羟基乙烷-1,1-二膦酸(HEDPA)和羟基乙烷膦酸(HEPA),作为质子传导的功能分子被引入到膜中。FT-IR和拉曼光谱研究表明杂化膜中存在膦酸基团,13 C和29 Si NMR证实杂化膜中通过水解和缩合反应形成了三维硅氧烷网络。DTA-TG分析表明,这些膜在高达200°C下是热稳定的。发现基于HEDPA的系统具有比基于HEPA的系统更高的质子传导率。杂化膜的质子传导率随着膦酸含量和温度的增加而增加,直到130°C。HEDPA/GPTMS/PhTES膜的电导率=1/1.6/0.4,在130°C、100%相对湿度和非增湿条件下分别为1.0×10 - 1和4.5×10 - 4Scm-1。
Proton conductive inorganic–organic hybrid membranes were synthesized from 3-glycidyloxypropyltrimethoxysiane (GPTMS), phenyltriethoxysilane (PhTES) and hydroxyalkylphosphonic acid. Two kinds of hydroxyalkylphosphonic acids, 1-hydroxyethane-1,1-diphosphonic acid (HEDPA) and hydroxyethanephosphonic acid (HEPA), were incorporated into the membranes as functional molecules for proton conduction. FT-IR and Raman studies revealed the presence of phosphonic acid groups in the hybrid membranes.13C and29Si NMR confirmed that a three-dimensional siloxane network was formed in the prepared hybrid membrane by hydrolysis and condensation reactions. DTA-TG analysis showed that these membranes were thermally stable up to 200°C. The HEDPA-based system was found to have higher proton conductivities than the HEPA-based one. The proton conductivities of the hybrid membranes increased with the phosphonic acid content and temperature up to 130°C. The conductivities of the HEDPA/GPTMS/PhTES membranes=1/1.6/0.4 were 1.0×10−1and 4.5×10−4Scm−1at 100% relative humidity and non-humidified conditions, respectively, at 130°C.