Dataset Information

In situ Raman study of the photoinduced behavior of dye molecules on TiO₂(hkl) single crystal surfaces.

ABSTRACT: In dye-sensitized solar cells (DSSCs), the TiO₂/dye interface significantly affects photovoltaic performance. However, the adsorption and photoinduced behavior of dye molecules on the TiO₂ substrate remains unclear. Herein, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) was used to study the adsorption and photoinduced behavior of dye (N719) molecules on different TiO₂(hkl) surfaces. On TiO₂(001) and TiO₂(110) surfaces, the in situ SHINERS and mass spectrometry results indicate S[double bond, length as m-dash]C bond cleavage in the anchoring groups of adsorbed N719, whereas negligible bond cleavage occurs on the TiO₂(111) surface. Furthermore, DFT calculations show the stability of the S[double bond, length as m-dash]C anchoring group on three TiO₂(hkl) surfaces in the order TiO₂(001) < TiO₂(110) < TiO₂(111), which correlated well with the observed photocatalytic activities. This work reveals the photoactivity of different TiO₂(hkl) surface structures and can help with the rational design of DSSCs. Thus, this strategy can be applied to real-time probing of photoinduced processes on semiconductor single crystal surfaces.

SUBMITTER: Zhang SP

PROVIDER: S-EPMC8159273 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

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In situ Raman study of the photoinduced behavior of dye molecules on TiO2(hkl) single crystal surfaces.

Zhang Sheng-Pei SP Lin Jia-Sheng JS Lin Rong-Kun RK Radjenovic Petar M PM Yang Wei-Min WM Xu Juan J Dong Jin-Chao JC Yang Zhi-Lin ZL Hang Wei W Tian Zhong-Qun ZQ Li Jian-Feng JF

Chemical science 20200417 25

In dye-sensitized solar cells (DSSCs), the TiO2/dye interface significantly affects photovoltaic performance. However, the adsorption and photoinduced behavior of dye molecules on the TiO2 substrate remains unclear. Herein, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) was used to study the adsorption and photoinduced behavior of dye (N719) molecules on different TiO2(hkl) surfaces. On TiO2(001) and TiO2(110) surfa ...[more]

PMID: 34094107

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Project description:Electro- and photochemical CO2 reduction (CO2R) is the quintessence of modern-day sustainable research. We report our studies on the electro- and photoinduced interfacial charge transfer occurring in a nanocrystalline mesoporous TiO2 film and two TiO2/iron porphyrin hybrid films (meso-aryl- and β-pyrrole-substituted porphyrins, respectively) under CO2R conditions. We used transient absorption spectroscopy (TAS) to demonstrate that, under 355 nm laser excitation and an applied voltage bias (0 to -0.8 V vs Ag/AgCl), the TiO2 film exhibited a diminution in the transient absorption (at -0.5 V by 35%), as well as a reduction of the lifetime of the photogenerated electrons (at -0.5 V by 50%) when the experiments were conducted under a CO2 atmosphere changing from inert N2. The TiO2/iron porphyrin films showed faster charge recombination kinetics, featuring 100-fold faster transient signal decays than that of the TiO2 film. The electro-, photo-, and photoelectrochemical CO2R performance of the TiO2 and TiO2/iron porphyrin films are evaluated within the bias range of -0.5 to -1.8 V vs Ag/AgCl. The bare TiO2 film produced CO and CH4 as well as H2, depending on the applied voltage bias. In contrast, the TiO2/iron porphyrin films showed the exclusive formation of CO (100% selectivity) under identical conditions. During the CO2R, a gain in the overpotential values is obtained under light irradiation conditions. This finding was indicative of a direct transfer of the photogenerated electrons from the film to absorbed CO2 molecules and an observed decrease in the decay of the TAS signals. In the TiO2/iron porphyrin films, we identified the interfacial charge recombination processes between the oxidized iron porphyrin and the electrons of the TiO2 conduction band. These competitive processes are considered to be responsible for the diminution of direct charge transfer between the film and the adsorbed CO2 molecules, explaining the moderate performances of the hybrid films for the CO2R.

Dataset Information

In situ Raman study of the photoinduced behavior of dye molecules on TiO₂(hkl) single crystal surfaces.

Publications

<i>In situ</i> Raman study of the photoinduced behavior of dye molecules on TiO<sub>2</sub>(<i>hkl</i>) single crystal surfaces.

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