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首页> 外文期刊>Chemistry: A European journal >Coupled Protonic and Electronic Conduction in the Molecular Conductor [2-(2-1H-Benzimidazolyl)-1H-benzimidazolium]-TCNQ
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Coupled Protonic and Electronic Conduction in the Molecular Conductor [2-(2-1H-Benzimidazolyl)-1H-benzimidazolium]-TCNQ

机译：分子导体[2-（2-1H-苯并咪唑基）-1H-苯并咪唑鎓] -TCNQ中的质子和电子耦合耦合

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摘要

A novel molecular based proton-electron mixed conductor, (H3BBIM~+)(TCNQ)(Cl~-)_0.5(H_2O) (1), where H3BBIM~+ is 2-(2-1H-benzimidazolyl)-1H-benzimidazolium and TCNQ is 7,7,8,8-tetrcyano-p-quinodimethane, was synthesized. The salt exhibited peculiar phase transitions as a result of proton-electron coupling phenomena within the crystal. Salt 1 is composed of a closed-shell H3BBIM~+ cation and an open-shell TCNQ anion radical, and was obtained by electrocrystallization in a buffered CH_3CN solution. Crystal 1 was constructed from the segregated uniform stakes of H3BBIM~+ and TCNQ. The regular stack of partially electron-transferred TCNQ~(-0.5) provided a one-dimensional electron-conducting column. Between the regular H3BBIM~~+ columns, a channel-like sequence of holes was formed at the side-by-side space that is filled with disordered Cl~- ions and H_2O molecules, and which offer a proton-conducting path. The electrical conductivity at room temperature (10 S cm~(-1)) was greater by a magnitude of four than the protonic conductivity (1 X 10~(-3) S cm~(-1)). Electronic conduction changed from metallic (T > 250 K) to semiconducting (250 > T > 100 K), then insulating (T < 100 K). Protonic conductivity was observed above 200 K. The continuous metal-semiconductor transition at 250 K is caused by the formation of the Cl~- superstructure, whereas the disappearance of protonic conductivity at 200 K is related to the rearrangement of the [Cl~--(H_2O)_2] sublattice within the channel. The magnetic susceptibility continuously shifted from Pauli paramagnetism (T > 250 K) to the one-dimensional linear Heisenberg antiferromagnetic chain (T < 250 K). Lattice dimerization in regular TCNQ columns was confirmed by the appearance of vibrational a_g mode at low temperatures. The strong localization of conduction electrons on each TCNQ dimer caused a Mott transition at 100 K. The melting and freezing of the [Cl~- - (H_2O)_2] sublattice within the channel was correlated to the conduction electrons on the TCNQ stack and the protonic conductivity.
机译：一种新型的基于分子的质子电子混合导体（H3BBIM〜+）（TCNQ）（Cl〜-）_ 0.5（H_2O）（1），其中H3BBIM〜+为2-（2-1H-苯并咪唑基）-1H-合成了苯并咪唑鎓和TCNQ为7,7,8,8-四氰基-对-喹二甲烷。由于晶体内的质子-电子耦合现象，该盐表现出独特的相变。盐1由闭壳的H3BBIM +阳离子和开壳的TCNQ阴离子自由基组成，是通过在缓冲的CH_3CN溶液中进行电结晶而获得的。晶体1是由H3BBIM〜+和TCNQ的分离的均匀桩构成的。部分电子转移的TCNQ〜（-0.5）的规则堆叠提供了一维电子传导柱。在常规的H3BBIM〜+柱之间，在并排的空间中形成了通道状的孔序列，其中充满了无序的Cl +和H_2O分子，并提供了质子传导路径。室温下的电导率（10 S cm〜（-1））比质子化的电导率（1 X 10〜（-3）S cm〜（-1）大四倍。电子传导从金属（T> 250 K）变为半导体（250> T> 100 K），然后变为绝缘（T <100 K）。在200 K以上观察到质子传导率。在250 K处连续的金属-半导体转变是由Cl〜-超结构的形成引起的，而在200 K时质子传导率的消失与[Cl〜-的重排有关（H_2O）_2]通道内的子晶格。磁化率连续从保利顺磁性（T> 250 K）转变为一维线性海森堡反铁磁链（T <250 K）。通过在低温下出现振动a_g模式，可以确认常规TCNQ色谱柱中的晶格二聚化。每个TCNQ二聚体上传导电子的强烈定位在100 K处引起Mott跃迁。通道内[Cl〜--（H_2O）_2]亚晶格的熔化和冻结与TCNQ叠层和衬底上的传导电子相关。质子传导性。

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