Bonhôte P, Gogniat E, Tingry S, Barbé C, Vlachopoulos N, Lenzmann F, Comte P, Grätzel M
Laboratoire de photonique et interfaces, Département de chimie, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland.
J Phys Chem B. 1998 Feb 26;102(9):1498-507. doi: 10.1021/jp972890j.
A monolayer of a phosphonated triarylamine adsorbed on nanocrystalline TiO2, ZrO2, or Al2O3 film deposited on conducting glass displays reversible electrochemical and electrochromic behavior although the redox potential of the electroactive molecules (0.80 V vs NHE) lies in the forbidden band of the semiconducting or insulating oxides. The mechanism of charge transport was found to involve hole injection from the conducting support followed by lateral electron hopping within the monolayer. The apparent diffusion coefficient ranged from 2.8 × 10(-12) m(2) s(-1) in the neat 1-ethyl-2-methylimidazolium bis(trifluoromethylsulfonyl)imide (EtMeIm(+)Tf2N(-)) to 1.1 × 10(-11) m(2) s(-1) in acetonitrile + 2 M EtMeIm(+)Tf2N(-). A percolation threshold for electronic conductivity was found at a surface coverage corresponding to 50% of a full monolayer.
吸附在沉积于导电玻璃上的纳米晶TiO₂、ZrO₂或Al₂O₃薄膜上的膦酸化三芳基胺单分子层表现出可逆的电化学和电致变色行为，尽管电活性分子的氧化还原电位（相对于标准氢电极0.80 V）处于半导体或绝缘氧化物的禁带中。发现电荷传输机制涉及从导电载体进行空穴注入，随后在单分子层内进行横向电子跳跃。表观扩散系数范围从在纯1-乙基-2-甲基咪唑鎓双（三氟甲基磺酰）亚胺（EtMeIm⁺Tf₂N⁻）中2.8×10⁻¹² m² s⁻¹到在乙腈 + 2 M EtMeIm⁺Tf₂N⁻中1.1×10⁻¹¹ m² s⁻¹。在对应于完整单分子层50%的表面覆盖度处发现了电子传导的渗流阈值。
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