The proton conduction mechanism in a material consisting of packed acids

The proton conduction mechanism in a material consisting of packed acids
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DOI:
10.1039/c4sc00952e
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发表时间:
2014-01-01
期刊:
影响因子:
8.4
通讯作者:
Yamaguchi, Takeo
Yamaguchi, Takeo
中科院分区:
化学1区
文献类型:
--
作者:
Ogawa, Takaya;Aonuma, Takashi;Yamaguchi, Takeo

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从材料科学到生物化学,酸-酸相互作用引起的质子传导是许多领域的重要课题。我们观察到在硫苯膦酸锆(ZrSPP)和磺化聚芳醚砜(spe)界面上由填充酸组成的材料具有独特的质子传导现象。复合材料中的质子被发现是活跃的,而水,一般的质子载体,保持不动。此外,复合材料的电导率高于ZrSPP和SPES的单独电导率之和,这可以归因于界面上存在堆积的酸。为了解释如此重要而有趣的质子行为,我们提出了一种基于从头计算结果的“填充酸机制”。在共质子传导过程中,质子在质子供体和受体之间的伪穿梭是破坏重定向现象的普遍事件,而重定向现象是与共质子传导相关的一个重要过程。根据我们的研究结果,我们可以推断,在填充的酸性物质中,酸-酸相互作用消除了伪穿梭(拦截)并促进了重新定向,从而导致了连续的质子传导。
Proton conduction due to acid-acid interactions is an important topic in a variety of fields, from materials science to biochemistry. We observed a distinctive proton conduction phenomenon for a material consisting of packed acids at the interface of zirconium sulphophenylphosphonate (ZrSPP) and sulphonated poly(arylene ether sulphone) (SPES). The proton in the composite was found to be active, while water, a general proton carrier, remained immobile. Moreover, the conductivity of the composite material was higher than the sum of the individual conductivities of ZrSPP and SPES, which can be attributed to the packed acids present at the interface. We propose a "packed-acid mechanism" based on the results of ab initio calculations in order to explain such a significant and interesting behaviour of protons. During common proton conduction, pseudo-shuttling of a proton between a proton donor and acceptor is a general event that disrupts the reorientation phenomenon, which is an important process associated with common proton conduction. Based on our results, it could be inferred that in packed acid materials, the acid-acid interaction eliminates the pseudo-shuttling (interception) and facilitates reorientation, resulting in successive proton conduction.