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1.
Nano Lett ; 15(6): 3833-9, 2015 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-25942281

RESUMO

Photoelectrochemical water splitting half reactions on semiconducting photoelectrodes have received much attention but efficient overall water splitting driven by a single photoelectrode has remained elusive due to stringent electronic and thermodynamic property requirements. Utilizing a tandem configuration wherein the total photovoltage is generated by complementary optical absorption across different semiconducting electrodes is a possible pathway to unassisted overall light-induced water splitting. Because of the low photovoltages generated by conventional photovoltaic materials (e.g., Si, CIGS), such systems typically consist of triple junction design that increases the complexity due to optoelectrical trade-offs and are also not cost-effective. Here, we show that a single solution processed organic-inorganic halide perovskite (CH3NH3PbI3) solar cell in tandem with a Fe2O3 photoanode can achieve overall unassisted water splitting with a solar-to-hydrogen conversion efficiency of 2.4%. Systematic electro-optical studies were performed to investigate the performance of tandem device. It was found that the overall efficiency was limited by the hematite's photocurrent and onset potential. To understand these limitations, we have estimated the intrinsic solar to chemical conversion efficiency of the doped and undoped Fe2O3 photoanodes. The total photopotential generated by our tandem system (1.87 V) exceeds both the thermodynamic and kinetic requirements (1.6 V), resulting in overall water splitting without the assistance of an electrical bias.


Assuntos
Compostos de Cálcio/química , Compostos Férricos/química , Óxidos/química , Fotólise , Luz Solar , Titânio/química , Água/química
2.
Adv Mater ; 28(37): 8191-8196, 2016 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-27417520

RESUMO

The family of solution-processed tin-based perovskites is demonstrated as a new and superior near-infrared gain medium. Due to the large electron-hole bimolecular recombination associated with tin and the reduced trap density with SnF2 treatment, these lead-free "green" perovskites yield stable coherent light emission extending to ≈1 µm at strikingly low thresholds.

3.
ACS Appl Mater Interfaces ; 6(20): 17661-7, 2014 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-25255739

RESUMO

A novel approach to produce earth-abundant Cu2FeSnS4 (CFTS) thin film using spray pyrolysis of nontoxic aqueous precursors followed by sulfurization is reported. The CFTS phase formation was confirmed by both Raman spectroscopy and X-ray diffraction techniques. Hall measurements of these films reveal p-type conductivity with good charge carrier density and mobilities appropriate for solar harvesting devices. To the best of our knowledge, this is the first report on the electrical properties of solution-processed Cu2FeSnS4 thin films estimated using Hall measurements. Dye-sensitized solar cells (DSSC) fabricated with CFTS thin film as a photocathode in iodine/iodide electrolyte exhibit good power conversion efficiency, 8.03%, indicating that CFTS would be a promising cheaper alternative to replace Pt as a counter electrode in DSSCs.

4.
ACS Appl Mater Interfaces ; 6(8): 5852-9, 2014 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-24702963

RESUMO

Here, we report a significant improvement of the photoelectrochemical (PEC) properties of hematite (α-Fe2O3) to oxidize water by doping with manganese. Hematite nanorods were grown on a fluorine-treated tin oxide (FTO) substrate by a hydrothermal method in the presence on Mn. Systematic physical analyses were performed to investigate the presence of Mn in the samples. Fe2O3 nanorods with 5 mol % Mn treatment showed a photocurrent density of 1.6 mA cm(-2) (75% higher than that of pristine Fe2O3) at 1.23 V versus RHE and a plateau photocurrent density of 3.2 mA cm(-2) at 1.8 V versus RHE in a 1 M NaOH electrolyte solution (pH 13.6). We attribute the increase in the photocurrent density, and thus in the oxygen evolving capacity, to the increased donor density resulting from Mn doping of the Fe2O3 nanorods, as confirmed by Mott-Schottky measurement, as well as the suppression of electron-hole recombination and enhancement in hole transport, as detected by chronoamperometry measurements.

5.
Adv Mater ; 26(41): 7122-7, 2014 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-25212785

RESUMO

Lead free perovskite solar cells based on a CsSnI3 light absorber with a spectral response from 950 nm is demonstrated. The high photocurrents noted in the system are a consequence of SnF2 addition which reduces defect concentrations and hence the background charge carrier density.

6.
Chem Commun (Camb) ; 49(94): 11089-91, 2013 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-24141601

RESUMO

A ZnO compact layer formed by electrodeposition and ZnO nanorods grown by chemical bath deposition (CBD) allow the processing of low-temperature, solution based and flexible solid state perovskite CH3NH3PbI3 solar cells. Conversion efficiencies of 8.90% were achieved on rigid substrates while the flexible ones yielded 2.62%.

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