Oriented Mesoporous Organosilica Films on Electrode: A New Class of Nanomaterials for Sensing
Oriented Mesoporous Organosilica Films on Electrode: A New Class of Nanomaterials for Sensing
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DOI：
10.1166/jnn.2009.se39
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发表时间：
2009-04-01
影响因子：
--
通讯作者：
Walcarius, Alain
中科院分区：
文献类型：
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作者：
Etienne, Mathieu;Goux, Aurelie;Walcarius, Alain
我们最近报道了一种新的电辅助自组装（EASA）方法，可以制造出高度有序的介孔二氧化硅薄膜，其介孔通道垂直于衬底（Nature Mater. 6,602(2007)）。如果可以在常规环境中引入可能与目标分析物相互作用的有机官能团，从而确保高可及性和快速的传质速率，那么沉积在电极表面的这种薄膜可以在传感应用中引起极大的兴趣。我们在此证明了以十六烷基三甲基溴化铵为模板，通过溶胶-凝胶共缩合途径一步电合成氨基丙基功能化介孔硅膜。在起始溶胶中，高达10%的氨基丙基三乙氧基硅烷前驱体保持了孔隙的取向。使用各种氧化还原探针(Ru(bpy)(3)(2+), FcEtOH, I-, Fe(CN)（6)(3-)）研究了膜中胺功能的存在会影响其对外部试剂的渗透性，并且发现缺乏介结构会显著阻碍质量传递过程。当应用于开路积累后的铜（II）伏安检测时，电极的响应受到功能化水平的极大影响，最佳传感器灵敏度是在保持介结构秩序的同时，在足够高的胺基数量之间的最佳平衡。
We have recently reported the possible fabrication of highly ordered mesoporous silica thin films with mesopore channels oriented perpendicularly to the underlying substrate, by means of novel electro-assisted self-assembly (EASA) method (Nature Mater. 6, 602 (2007)). Such films deposited on an electrode surface can be of great interest in sensing applications if one could introduce organo-functional groups likely to interact with target analytes in a regular environment ensuring great accessibility and fast mass transfer rates. We demonstrate here that aminopropyl-functionalized mesoporous silica films can be electrogenerated in one step by the sol-gel co-condensation route using cetyltrimethylammonium bromide as template. The orientation of the pore is maintained up to 10% aminopropyltriethoxysilane precursor in the starting sol. The presence of amine functions into the film affects its permeability to external reagents, as studied using various redox probes (Ru(bpy)(3)(2+), FcEtOH, I-, Fe(CN)(6)(3-)), and the lack of mesostructuration was found to hinder dramatically mass transport processes. When applied to the voltammetric detection of copper(II) subsequent to open-circuit accumulation, the response of the electrode was greatly affected by the functionalization level, the optimal sensor sensitivity being defined from the best compromise between an amount of amine groups high enough while maintaining mesostructural order.