Photoelectric performance of TiO2 nanotube array photoelectrodes sensitized with CdS0.54Se0.46 quantum dots

doi:10.1016/j.apsusc.2015.07.169

Applied Surface Science

Volume 355, 15 November 2015, Pages 1279-1288

https://doi.org/10.1016/j.apsusc.2015.07.169 Get rights and content

Highlights

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CdSSe quantum dots were successfully tethered to titania nanotubes.
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XRD showed the stoichiometry of the quantum dots to be CdS_0.54Se_0.46.
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The optimal film led to an 11-fold higher photocurrent than unmodified TiO₂ film.

Abstract

The photoelectrochemical performance of CdSSe quantum dots tethered to a framework of vertically oriented titania (TiO₂) nanotubes was studied. The TiO₂/CdSSe framework demonstrated improved charge transfer due to its unique band edge structure, thus validating the higher photocurrent generation. The composite film led to an 11-fold enhancement in comparison to the control TiO₂ film, implying that the ternary quantum dots and the nanotubular structure of TiO₂ work in tandem to promote charge separation and favorably impact photoelectrochemical performance. Further, the results also suggest that structural and optoelectronic properties of TiO₂ films are significantly affected by the thicknesses of the CdSSe layer.

Introduction

Semiconductor quantum dots (QDs) with tunable band gaps offer a solution to the problems associated with the use of conventional organic dyes in solar devices by harvesting a wider portion of the solar spectrum [1], [2]. Quantum dots show high emission quantum yield, narrow and symmetric emission peaks, and tunable, size-dependent band gaps [3]. In addition, the high photostability and chemical stability of QDs compared to organic dyes enables their use in the design of photovoltaic devices that require long exposure times. It has been demonstrated that quantum confinement greatly affects the width of the optical band gap and associated spectral features in semiconductor nanocrystals. Spatial confinement results in multi-exciton generation (MEG), also referred as Inverse Auger effect, which largely affects the power conversion efficiency of quantum dots-sensitized solar cells (QDSSCs) [4], [5]. However, the performance of QDSSCs is still lower than that of their dye-sensitized solar cells (DSSCs) counterpart [3], in spite of the fact that the theoretical maximum conversion efficiency of QDSSCs (44%) is considerably higher than that of DSSCs (31%) [6]. Therefore, attempts are being made to improve the efficiency of QDSSCs.

The most widely studied photoanode materials are oxide semiconductors, particularly TiO₂, since it is stable under visible light illumination. Until recently, the sensitization of TiO₂ with semiconductor QDs has been investigated mainly with titania nanoparticulate films. Such films, however, suffer from structural disorders due to grain boundaries, which impede the charge separation efficiency and charge transport through the material. These drawbacks render TiO₂ particulate films less efficient as photoanodes while, TiO₂ nanotubes arrays (NTA), with their unique properties, offer improved charge transfer characteristics. Titania nanotube arrays have advantages over particulate films such as cheap and facile fabrication technique, high surface area to volume ratio, tunable dimensions (pore size and tube length), and the 1D architecture furnishes less impeded pathways for electron transfer and transport [7], [8].

As sensitizers, cadmium chalcogenide (CdX, X = S, Se or Te) QDs have attracted considerable attention in QDSSC research over the last few years [9], [10], [11], [12], [13], [14], [15], [16], [17], [18], [19], [20]. It has been noted that CdX absorb photons efficiently because these have a bulk material band gap greater than 1.3 eV; band gaps for CdS, CdSe and CdTe are 2.25 eV, 1.73 eV, and 1.49 eV, respectively. By altering the size of the QDs, the band gap can be tuned further to match a desired band gap range. While considerable studies have been conducted on co-sensitization of TiO₂ with CdS and CdSe [20], [21], [22], [23], [24], [25], [26], [27], [28], [29], [30], only few studies can be found on CdSSe/TiO₂ NTA heterostructure [31], [32], [33]. Chong et al. [31] studied CdSSe quantum dots attached to TiO₂ nanobelts synthesized by hydrothermal route and found remarkable enhancement in photocurrent with good reproducibility for sensitized samples. Luo et al. [32] synthesized photoelectrodes with nanorods of CdS, CdSe, and CdSeS deposited onto TiO₂ nanorod arrays and found that the TiO₂/CdSeS heterostructure was the most stable. Park et al. [33] demonstrated the fabrication of regular arrays of TiO₂ nanotubes anchored with ZnS/CdSSe/CdS quantum dots by the SILAR method, which exhibited a power conversion efficiency of 4.67% in a QDSSC configuration.

The current study presents a simple, yet efficient, route for the synthesis of TiO₂ NTA heterostructure in conjunction with quantum sized CdSSe clusters. A balance between energetics and kinetics of the system has been realized by means of alignment of the conduction band edges, where, the conduction band (CB) of CdSSe lies above the CB of TiO₂. The morphology and crystallinity of the CdSSe layer was characterized and correlated with photoelectrochemical activity.

Section snippets

Experimental

Self-organized TiO₂ nanotube arrays were synthesized by anodic oxidation of an ultrasonically cleaned Ti foil. The anodization was carried out in an organic electrolyte containing 0.5 wt% NH₄F at 40 V (DC) for 1 h. The details of the experiment can be found elsewhere [34], [35]. After anodization, the films were rinsed with isopropyl alcohol to remove any particulates on top of the film. The film was then annealed in air at 450 °C for 2 h.

CdSSe nanocrystals were deposited on TiO₂ NTAs using the

Structural and optical characterization

UV–visible absorption spectra of prepared photoelectrodes were obtained with a Shimadzu UV-2401PC UV–vis diffuse reflectance spectrophotometer. BaSO₄ was used as the reflectance standard in the wavelength range of 200–800 nm. The surface morphologies of TiO₂ NTAs and CdSSe-deposited TiO₂ NTA films were examined by a Hitachi S-4800 scanning electron microscope equipped with an energy dispersive spectrometer (Oxford EDS system). Transmission electron micrographs were recorded using a JEOL

Optical absorption study

The UV–visible light absorbance properties of TiO₂ NTA/CdSSe (n) photoanodes are depicted in Fig. 1. The effect of the number of deposition layers (n = 5, 7 and 9 cycles) and post-synthesis annealing temperature (300 and 400 °C) on the optical performance of the modified electrodes was studied and compared with unsensitized TiO₂ NTAs (Fig. 1). Plain TiO₂ NTA film shows an absorption edge at 380 nm, corresponding to the bandgap of the anatase phase of titania [36], [37]. An additional feature (broad

Conclusions

The CdSSe-sensitized TiO₂ photoelectodes were synthesized using a convenient SILAR process. The influence of the thickness of the CdSSe and the annealing temperature on photoelectrochemical response was studied. Photovoltaic characteristic of TNTAs exhibit substantial improvement upon sensitization and again with the increase in CdSSe layer thickness. For films with 9 cycle of thickness sensitization and annealed at 400 °C, sensitization was found to result in a 11-fold enhancement in

Acknowledgements

The authors sincerely thank Dr. Wen-Ming Chien for technical assistance regarding XRD measurements and Kodi Summers for assistance with preparation of samples. We also thank Dr. Mojtaba Ahmadiantehrani for obtaining the TEM images. This work was funded by Department of Energy under contracts DE-FC36-06-GO86066 and DE-EE0003158.

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Citation Excerpt :
However, the synthesis of CdS1-xSex alloy QDs or nanocrystals for QDSSCs involved three major techniques: the chemical bath deposition (CBD), the successive ion layer absorption and reaction (SILAR) [15], and the hot-injection solvothermal synthesis (HISS) [25]. When SILAR route was employed to prepare CdS1-xSex alloy QDs, not only CdS and CdSe layers were alternately deposited to form CdS1-x Sex solid solution or CdS1-xSex alloy [26–28], but also a mixture solution containing S2− and Se2− was involved [29–31]. In addition, the mixture precursor containing Cd2+, S2− and Se2− was also used to deposit CdS1-x Sex alloy QDs by a one-pot reaction in CBD and HISS.
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Photoelectric performance of TiO2 nanotube array photoelectrodes sensitized with CdS0.54Se0.46 quantum dots

Highlights

Abstract

Introduction

Section snippets

Experimental

Structural and optical characterization

Optical absorption study

Conclusions

Acknowledgements

Renew. Sustain. Energy Rev.

Chem. Phys. Lett.

Electrochem. Commun.

Electrochem. Commun.

Electrochim. Acta

Appl. Surf. Sci.

Appl. Surf. Sci.

Electrochim. Acta

Appl. Surf. Sci.

Electrochim. Acta

Sol. Energy Mater. Sol. Cells

Appl. Surf. Sci.

Electrochim. Acta

Int. J. Hydrogen Energy

Thin Solid Films

Electrochim. Acta

Electrochim. Acta

Electrochim. Acta

Appl. Surf. Sci.

Electronic wave functions in semiconductor clusters: experiment and theory

J. Phys. Chem.

Perspectives on the physical chemistry of semiconductor nanocrystals

J. Phys. Chem.

High efficiency carrier multiplication in PbSe nanocrystals: implications for solar energy conversion

Phys. Rev. Lett.

J. Appl. Phys.

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J. Phys. Chem. C

CuInS2 quantum dot-sensitized TiO2 nanorod array photoelectrodes: synthesis and performance optimization

Nanoscale Res. Lett.

Photoelectrochemical behavior of thin cadmium selenide and coupled titania/cadmium selenide semiconductor films

J. Phys. Chem.

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Nanotechnology

CdS/CdSe co-sensitized TiO2 photoelectrode for efficient hydrogen generation in a photoelectrochemical cell

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Photoelectric performance of TiO₂ nanotube array photoelectrodes sensitized with CdS_0.54Se_0.46 quantum dots

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