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Investigating Charge Transfer in Functionalized Mesoporous EISA–SnO2 Films
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2017-10-09 00:00:00 , DOI: 10.1021/acs.jpcc.7b07071
Wael Hamd 1 , Christel Laberty-Robert 2 , François Lambert 3 , Cyrille Costentin 1 , Benoît Limoges 1 , Véronique Balland 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2017-10-09 00:00:00 , DOI: 10.1021/acs.jpcc.7b07071
Wael Hamd 1 , Christel Laberty-Robert 2 , François Lambert 3 , Cyrille Costentin 1 , Benoît Limoges 1 , Véronique Balland 1
Affiliation
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Semiconductive transparent thin films of periodically organized nanostructured SnO2 were prepared on flat conductive ITO substrates by evaporation-induced self-assembly (EISA) under different dip-coating regimes and then functionalized by two redox-active chromophores, i.e., the flavin mononucleotide (FMN) able to reversibly exchange 2 e– and 2 H+ and the [OsII(bpy)2(4,4′-CH2PO3H2-bpy)]2+ complex (OsP) involving a fast and reversible one-electron transfer. The redox behavior of these two chemisorbed chromophores was investigated by cyclic voltammetry and cyclic voltabsorptometry. On account of the distinct formal potential of the two redox chromophores relative to the position of the lower conduction band edge of SnO2, the heterogeneous electron transfer was observed to be either reversible (FMN) or irreversible (OsP). In the case of the OsP-functionalized SnO2 electrode, quantitative analysis of the cyclic voltabsorptograms was achieved within the framework of our previously proposed kinetic model of charge transfer/transport in mesoporous semiconductive films (Renault et al. Phys. Chem. Chem. Phys. 2015, 17, 10592), allowing for direct comparison between EISA–TiO2 and EISA–SnO2 electrodes. It is notably shown that the interfacial electron transfer between the adsorbed redox chromophore and the SnO2 interface is the rate-determining process under our experimental conditions. It is additionally demonstrated that the electrons trapped in the low-energy surface states of EISA–SnO2 can directly participate in the interfacial electron transfer, a behavior that strongly contrasts that which we had previously found at EISA–TiO2 electrodes (i.e., wherein only electrons from the conduction band were involved in the interfacial electron transfer).
中文翻译:
研究功能化介孔EISA–SnO 2膜中的电荷转移
在不同的浸涂方式下,通过蒸发诱导自组装(EISA)在平面导电ITO基板上制备周期性组织的纳米结构SnO 2的半透明半导体薄膜,然后通过两个氧化还原活性生色团即黄素单核苷酸(FMN)进行功能化)能够可逆地交换2 e –和2 H +和[Os II(bpy)2(4,4'-CH 2 PO 3 H 2 -bpy)] 2+复杂(OsP),涉及快速且可逆的单电子转移。通过循环伏安法和循环伏安法研究了这两种化学吸附的生色团的氧化还原行为。由于两个氧化还原发色团相对于SnO 2的较低导带边缘的位置具有不同的形式势,因此观察到异质电子转移是可逆的(FMN)或不可逆的(OsP)。在OsP功能化的SnO 2电极的情况下,循环伏安曲线图的定量分析是在我们先前提出的介孔半导体薄膜中电荷转移/迁移动力学模型的框架内完成的(Renault等人, Phys。Chem。Chem。Phys。 。 2015年, 17, 10592),可以直接比较EISA-TiO 2和EISA-SnO 2电极。值得注意的是,在我们的实验条件下,吸附的氧化还原生色团与SnO 2界面之间的界面电子转移是决定速率的过程。此外,还证明了陷于EISA-SnO 2低能表面态的电子可以直接参与界面电子转移,这种行为与我们先前在EISA-TiO 2电极上发现的行为形成了鲜明的对比(即,其中只有来自导带的电子才参与界面电子转移。
更新日期:2017-10-10
中文翻译:
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研究功能化介孔EISA–SnO 2膜中的电荷转移
在不同的浸涂方式下,通过蒸发诱导自组装(EISA)在平面导电ITO基板上制备周期性组织的纳米结构SnO 2的半透明半导体薄膜,然后通过两个氧化还原活性生色团即黄素单核苷酸(FMN)进行功能化)能够可逆地交换2 e –和2 H +和[Os II(bpy)2(4,4'-CH 2 PO 3 H 2 -bpy)] 2+复杂(OsP),涉及快速且可逆的单电子转移。通过循环伏安法和循环伏安法研究了这两种化学吸附的生色团的氧化还原行为。由于两个氧化还原发色团相对于SnO 2的较低导带边缘的位置具有不同的形式势,因此观察到异质电子转移是可逆的(FMN)或不可逆的(OsP)。在OsP功能化的SnO 2电极的情况下,循环伏安曲线图的定量分析是在我们先前提出的介孔半导体薄膜中电荷转移/迁移动力学模型的框架内完成的(Renault等人, Phys。Chem。Chem。Phys。 。