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1.
Sb2Se3, a V2‐VI3 compound semiconductor, has attracted extensive research attention in photovoltaics due to its non‐toxicity, low cost and earth‐abundant constituents. Herein, a combinatorial approach to optimize the performance of TiO2/Sb2Se3 thin film photovoltaics is employed. By simultaneously conducting a series of experiments in parallel rather than one after another, combinatorial strategy increases experimental throughput and reduces personnel costs. Key parameters such as TiO2 thickness, post‐annealing temperature and Sb2Se3 thickness are identified as 65 nm, 450 °C and 850 nm through the combinatorial approach. Finally, in combination with (NH4)2S back surface cleaning, TiO2/Sb2Se3 solar cells with 5.6% efficiency and decent stability are obtained, showcasing the power of high‐throughput strategy for accelerating the optimization of Sb2Se3 photovoltaics.  相似文献   

2.
Overcoming ionic diffusion limitations is essential for the development of high‐efficiency dye‐sensitized solar cells based on cobalt redox mediators. Here, improved mass transport is reported for photoanodes composed of mesoporous TiO2 beads of varying pore sizes and porosities in combination with the high extinction YD2‐o‐C8 porphyrin dye. Compared to a photoanode made of 20 nm‐sized TiO2 particles, electrolyte diffusion through these films is greatly improved due to the large interstitial pores between the TiO2 beads, resulting in up to 70% increase in diffusion‐limited current. Simultaneously, transient photocurrent measurements reveal no mass transport limitations for films of up to 10 μm thickness. In contrast, standard photoanodes made of 20 nm‐sized TiO2 particles show non‐linear behavior in photocurrent under 1 sun illumination for a film thickness as low as 7 μm. By including a transparent thin mesoporous TiO2 underlayer in order to reduce optical losses at the fluorine‐doped tin oxide (FTO)‐TiO2 interface, an efficiency of 11.4% under AM1.5G 1 sun illumination is achieved. The combination of high surface area, strong scattering behavior, and high porosity makes these mesoporous TiO2 beads particularly suitable for dye‐sensitized solar cells using bulky redox couples and/or viscous electrolytes.  相似文献   

3.
Novel thin film composite photocathodes based on device‐grade Cu(In,Ga)Se2 chalcopyrite thin film absorbers and transparent conductive oxide Pt‐implemented TiO2 layers on top are presented for an efficient and stable solar‐driven hydrogen evolution. Thin films of phase‐pure anatase TiO2 are implemented with varying Pt‐concentrations in order to optimize simultaneously i) conductivity of the films, ii) electrocatalytic activity, and iii) light‐guidance toward the chalcopyrite. Thereby, high incident‐photon‐to‐current‐efficiencies of more than 80% can be achieved over the full visible light range. In acidic electrolyte (pH 0.3), the most efficient Pt‐implemented TiO2–Cu(In,Ga)Se2 composite electrodes reveal i) photocurrent densities up to 38 mA cm?2 in the saturation region (?0.4 V RHE, reversible hydrogen electrode), ii) 15 mA cm?2 at the thermodynamic potential for H2‐evolution (0 V RHE), and iii) an anodic onset potential shift for the hydrogen evolution (+0.23 V RHE). It is shown that the gradual increase of the Pt‐concentration within the TiO2 layers passes through an efficiency‐ and stability‐maximum of the device (5 vol% of Pt precursor solution). At this maximum, optimized light‐incoupling into the device‐grade chalcopyrite light‐absorber as well as electron conductance properties within the surface layer are achieved while no degradation are observed over more than 24 h of operation.  相似文献   

4.
TiOx (x < 2) nanoparticles with tunable colors from white to gray to blue–gray to black are synthesized by magnesium (Mg) reduction of white P25 TiO2 nanocrystals followed by removal of excess Mg with aqueous HCl and distilled water. Increasing amounts of Mg smoothly decrease the oxygen content in TiOx which is responsible for the gradual increase in light absorption and concomitant darkening of its color from white to black with decreasing values of x. The as‐synthesized TiOx nanoparticles are spin‐coated onto the surface of a stainless steel mesh followed by surface superhydrophobization in order to test their performance as a solar water evaporator. Results from the tests show that the black TiOx efficiently generates water vapor with a solar thermal conversion efficiency as high as 50% under solar‐simulated light irradiance at an intensity of 1000 W m–2 (1 Sun). Moreover, TiOx nanoparticles have inherent advantages over other materials used for solar water desalination, such as their tunable light absorption, low‐cost, low‐toxicity, superhydrophobicity, and chemical stability.  相似文献   

5.
Organic–inorganic hybrid perovskite solar cells (PVSCs) have become the front‐running photovoltaic technology nowadays and are expected to profoundly impact society in the near future. However, their practical applications are currently hampered by the challenges of realizing high performance and long‐term stability simultaneously. Herein, the development of inverted PVSCs is reported based on low temperature solution‐processed CuCrO2 nanocrystals as a hole‐transporting layer (HTL), to replace the extensively studied NiOx counterpart due to its suitable electronic structure and charge carrier transporting properties. A ≈45 nm thick compact CuCrO2 layer is incorporated into an inverted planar configuration of indium tin oxides (ITO)/c‐CuCrO2/perovskite/[6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM)/bathocuproine (BCP)/Ag, to result in the high steady‐state power conversion efficiency of 19.0% versus 17.1% for the typical low temperature solution‐processed NiOx‐based devices. More importantly, the optimized CuCrO2‐based device exhibits a much enhanced photostability than the reference device due to the greater UV light‐harvesting of the CuCrO2 layer, which can efficiently prevent the perovskite film from intense UV light exposure to avoid associated degradation. The results demonstrate the promising potential of CuCrO2 nanocrystals as an efficient HTL for realizing high‐performance and photostable inverted PVSCs.  相似文献   

6.
A crucial issue regarding emerging nanotechnologies remains the up‐scaling of new functional nanostructured materials towards their implementation in high performance applications on a large scale. In this context, we demonstrate high efficiency solid‐state dye‐sensitized solar cells prepared from new porous TiO2 photoanodes based on laser pyrolysis nanocrystals. This strategy exploits a reduced number of processing steps as well as non‐toxic chemical compounds to demonstrate highly porous TiO2 films. The possibility to easily tune the TiO2 nanocrystal physical properties allows us to demonstrate all solid‐state dye‐sensitized devices based on a commercial benchmark materials (organic indoline dye and molecular hole transporter) presenting state‐of‐the‐art performance comparable with reference devices based on a commercial TiO2 paste. In particular, a drastic improvement in pore infiltration, which is found to balance a relatively lower surface area compared to the reference electrode, is evidenced using laser‐synthesized nanocrystals resulting in an improved short‐circuit current density under full sunlight. Transient photovoltage decay measurements suggest that charge recombination kinetics still limit device performance. However, the proposed strategy emphasizes the potentialities of the laser pyrolysis technique for up‐scaling nanoporous TiO2 electrodes for various applications, especially for solar energy conversion.  相似文献   

7.
Understanding the degradation mechanisms of photoelectrodes and improving their stability are essential for fully realizing solar‐to‐hydrogen conversion via photo‐electrochemical (PEC) devices. Although amorphous TiO2 layers have been widely employed as a protective layer on top of p‐type semiconductors to implement durable photocathodes, gradual photocurrent degradation is still unavoidable. This study elucidates the photocurrent degradation mechanisms of TiO2‐protected Sb2Se3 photocathodes and proposes a novel interface‐modification methodology in which fullerene (C60) is introduced as a photoelectron transfer promoter for significantly enhancing long‐term stability. It is demonstrated that the accumulation of photogenerated electrons at the surface of the TiO2 layer induces the reductive dissolution of TiO2, accompanied by photocurrent degradation. In addition, the insertion of the C60 photoelectron transfer promoter at the Pt/TiO2 interface facilitates the rapid transfer of photogenerated electrons out of the TiO2 layer, thereby yielding enhanced stability. The Pt/C60/TiO2/Sb2Se3 device exhibits a high photocurrent density of 17 mA cm?2 and outstanding stability over 10 h of operation, representing the best PEC performance and long‐term stability compared with previously reported Sb2Se3‐based photocathodes. This research not only provides in‐depth understanding of the degradation mechanisms of TiO2‐protected photocathodes, but also suggests a new direction to achieve durable photocathodes for photo‐electrochemical water splitting.  相似文献   

8.
The high thermal stability and facile synthesis of CsPbI2Br all‐inorganic perovskite solar cells (AI‐PSCs) have attracted tremendous attention. As far as electron‐transporting layers (ETLs) are concerned, low temperature processing and reduced interfacial recombination centers through tunable energy levels determine the feasibility of the perovskite devices. Although the TiO2 is the most popular ETL used in PSCs, its processing temperature and moderate electron mobility hamper the performance and feasibility. Herein, the highly stable, low‐temperature processed MgZnO nanocrystal‐based ETLs for dynamic hot‐air processed Mn2+ incorporated CsPbI2Br AI‐PSCs are reported. By holding its regular planar “n–i–p” type device architecture, the MgZnO ETL and poly(3‐hexylthiophene‐2,5‐diyl) hole transporting layer, 15.52% power conversion efficiency (PCE) is demonstrated. The thermal‐stability analysis reveals that the conventional ZnO ETL‐based AI‐PSCs show a serious instability and poor efficiency than the Mg2+ modified MgZnO ETLs. The photovoltaic and stability analysis of this improved photovoltaic performance is attributed to the suitable wide‐bandgap, low ETL/perovskite interface recombination, and interface stability by Mg2+ doping. Interestingly, the thermal stability analysis of the unencapsulated AI‐PSCs maintains >95% of initial PCE more than 400 h at 85 °C for MgZnO ETL, revealing the suitability against thermal degradation than conventional ZnO ETL.  相似文献   

9.
As a promising alternative, inorganic perovskite nanocrystals allow reinforced stability of photovoltaic device. Unfortunately, directly assembling these nanocrystals into film is uncontrollable. Instead, in situ assembling technology under low temperature in open air is attractive but limited due to the tendency of nonperovskite transition. The adverse shell ligands and unstable core lattices are known as the fundamental problems. In order to address this issue, here proposed is a rational core–shell design: 1) with respect to ligands, a new one, 4‐fluorophenethylammonium iodide, is used to enhance bonding force and charge coupling between ligands and nanocrystals; 2) with respect to lattices, a novel compound H2PbI4 is employed to assist divalent ion (Mn2+) doping into perovskite lattices. By low temperature in situ processing CsPbI3 quasi‐nanocrystal film, the highest power conversion efficiency of 13.4% for p‐i‐n solar cells is achieved, which retains 92% after 500 h in ambient air. The current study underlines the significance of rational hierarchical design of inorganic perovskite nanocrystals, especially for low temperature in situ processable electronic devices.  相似文献   

10.
Environmental friendly aqueous‐processed solar cells have become one of the most promising candidates for the next‐generation photovoltaic devices. Researchers have made lots of progress in designing active materials with novel structures, manipulating the defects in active materials, optimizing device architecture, etc. However, it has long been a challenge to control the width of the depletion region and enhance carrier extraction ability. Fabrication of a thick bulk heterojunction (BHJ) film is an effective strategy to address these issues but difficult to realize. Herein, the thicker BHJ film of ZnO:CdTe is successfully fabricated and incorporated into CdTe‐poly(p‐phenylenevinylene) hybrid solar cells. As expected, this BHJ film enhances light absorption, extends the width of the depletion region, prolongs carrier lifetime, and promotes carrier extraction ability. Moreover, the electron transport layer of sol–gel ZnO with excellent transmittance and electrical conductivity boosts electron generation, transport, and injection, which further improves the device performance. As a result, the highest short current density (Jsc) of 19.5 mA cm?2, power conversion efficiency of 6.51%, and the widest depletion region (177 nm) are obtained in aqueous‐processed hybrid solar cells.  相似文献   

11.
Efficient sunlight‐driven water splitting devices can be achieved by pairing two absorbers of different optimized bandgaps in an optical tandem design. With tunable absorption ranges and cell voltages, organic–inorganic metal halide perovskite solar cells provide new opportunities for tailoring top absorbers for such devices. In this work, semitransparent perovskite solar cells are developed for use as the top cell in tandem with a smaller bandgap photocathode to enable panchromatic harvesting of the solar spectrum. A new CuInxGa1‐xSe2 multilayer photocathode is designed, exhibiting excellent performance for photoelectrochemical water reduction and representing a near‐ideal bottom absorber. When pairing it below a semitransparent CH3NH3PbBr3‐based solar cell, a solar‐to‐hydrogen efficiency exceeding 6% is achieved, the highest value yet reported for a photovoltaic–photoelectrochemical device utilizing a single‐junction solar cell as the bias source under one sun illumination. The analysis shows that the efficiency can reach more than 20% through further optimization of the perovskite top absorber.  相似文献   

12.
Recent research on fabricating scaffold‐type perovskite solar cells on plastic substrates has reported noteworthy progress in replacing the high‐temperature processing of TiO2 scaffolds and compact layers with various low‐temperature processes. Herein, recent progress in the laboratory is reported regarding the development of electrodeposited TiOx compact layers and brookite TiO2 scaffolds, both of which can be processed under 150 °C without greatly sacrificing their photovoltaic performance. Through systematic characterization of device properties and careful optimization of the fabrication conditions, a record‐high 15.76% power conversion efficiency of a plastic TiO2 scaffold‐type perovskite solar cell is demonstrated. In addition, bending durability and preliminary stability tests on this plastic perovskite solar cell show promising results and indicate clear directions for future improvement.  相似文献   

13.
Regulating the chemical/physical features of solution processed metal halide perovskite films by integrating sub‐10 nm nanocrystals is a highly promising strategy to advance their outstanding optoelectronic performance. However, significant challenges remain for the universal embedding of the well‐defined nanocrystals in the film matrix. By generating nanocrystals in desired solvents via pulsed laser irradiation in liquid, the authors demonstrate the effective decoration of sub‐10 nm nanocrystals in perovskite films for enhanced optoelectronic performance. It is believed that this improved performance is due to the modification of the widely adopted “antisolvent” to a novel “anti‐colloidal‐solution” (ACS). Exemplified by a typical ACS; carbon dots in chlorobenzene, its encouraging superiority in regulating, not only the films morphology, but also the electronic structure, is demonstrated. This results in perovskite solar cells with a champion efficiency of 21.41% as well as a pronounced stability over 5000 h in relative humidity of 40%. The capability of nanocrystal embedding for boosted photovoltaic performance is further exploited by employing other laser generated ACSs. Such a strategy may open up a route to regulating hybrid perovskite film performance via nanocrystal embedding for photovoltaics or even beyond optoelectronic applications.  相似文献   

14.
Recent advances in the efficiency of crystalline silicon (c‐Si) solar cells have come through the implementation of passivated contacts that simultaneously reduce recombination and resistive losses within the contact structure. In this contribution, low resistivity passivated contacts are demonstrated based on reduced titania (TiOx) contacted with the low work function metal, calcium (Ca). By using Ca as the overlying metal in the contact structure we are able to achieve a reduction in the contact resistivity of TiOx passivated contacts of up to two orders of magnitude compared to previously reported data on Al/TiOx contacts, allowing for the application of the Ca/TiOx contact to n‐type c‐Si solar cells with partial rear contacts. Implementing this contact structure on the cell level results in a power conversion efficiency of 21.8% where the Ca/TiOx contact comprises only ≈6% of the rear surface of the solar cell, an increase of 1.5% absolute compared to a similar device fabricated without the TiOx interlayer.  相似文献   

15.
Sequential series multijunction dye‐sensitized solar cells (SSM‐DSCs) can power solar‐to‐fuel processes with a single illuminated area device. Dye selection and strategies limiting photon losses are critical in SSM‐DSC devices for higher performance systems. Herein, an efficient and readily applicable spin coating protocol on glass surfaces with an antireflective fluoropolymer (CYTOP) is applied to an SSM‐DSC architecture. Combining CYTOP with the use of an immersion oil between glass spacers in a three subcell SSM‐DSC with judiciously selected TiO2 photoanode sensitizers and thicknesses, an overall power conversion efficiency (PCE) of 10.1% is obtained with an output of 2.3 V. Without external bias, this SSM‐DSC configuration shows an impressive overall solar‐to‐fuel conversion efficiency of 6% when powering IrO2 and Au2O3 electrocatalysts for CO2 and H2O to CO and H2 conversion in aqueous solution. The role of CYTOP, immersion oil, sensitizer selection, and film thickness on SSM‐DSC devices is discussed along with the stability of this system.  相似文献   

16.
Electrogenerated chemiluminescence (ECL) of thiol‐capped CdTe quantum dots (QDs) in aqueous solution was greatly enhanced by PDDA‐protected graphene (P‐GR) film that were used for the sensitive detection of H2O2. When the potential was cycled between 0 and ?2.3 V, two ECL peaks were observed at ?1.1 (ECL‐1) and ?1.4 V (ECL‐2) in pH 11.0, 0.1 M phosphate buffer solution (PBS), respectively. The electron‐transfer reaction between individual electrochemically‐reduced CdTe nanocrystal species and oxidant coreactants (H2O2 or reduced dissolved oxygen) led to the production of ECL‐1. While mass nanocrystals packed densely in the film were reduced electrochemically, assembly of reduced nanocrystal species reacted with coreactants to produce an ECL‐2 signal. ECL‐1 showed higher sensitivity for the detection of H2O2 concentrations than that of ECL‐2. Further, P‐GR film not only enhanced ECL intensity of CdTe QDs but also decreased its onset potential. Thus, a novel CdTe QDs ECL sensor was developed for sensing H2O2. Light intensity was linearly proportional to the concentration of H2O2 between 1.0 × 10?5 and 2.0 x 10‐7 mol L?1 with a detection limit of 9.8 x 10?8 mol L?1. The P‐GR thin‐film modified glassy carbon electrode (GCE) displayed acceptable reproducibility and long‐term stability. Copyright © 2012 John Wiley & Sons, Ltd.  相似文献   

17.
Novel approaches for the fabrication of dye‐sensitized solar cells (DSCs) are reported in which all the main constituent materials are processed by laser radiation. In addition to laser sintering of the nanocrystalline TiO2 film it is shown that lasers can be successfully utilized for nc‐TiO2 film patterning, platinization of the counter‐electrode, and efficient gasket sealing. All the mentioned processes are optimized and utilized for the fabrication of the first efficient and durable all‐laser‐based DSCs. Under one sun A.M. 1.5 illumination the power conversion efficiency (PCE) is 5.3% (6.2% unmasked) and also greater than or equal to the PCE of the cell fabricated with the same materials set but processed using conventional procedures (5.2%). These results open up a new scenario for DSC technology, i.e., that of setting up an entire, laser‐based, three‐step DSC pilot production line with tangible advantages in terms of effective processing, automation, large area scalability, and embedded energy.  相似文献   

18.
Recent advances in solar water splitting by using BiVO4 as a photoanode have greatly optimized charge carrier and reaction dynamics, but relatively wide bandgap and poor photostability are still bottlenecks. Here, an excellent photoanode of black BiVO4@amorphous TiO2?x to tackle both problems is reported. Its applied bias photon‐to‐current efficiency for solar water splitting is up to 2.5%, which is a new record for a single oxide photon absorber. This unique core–shell structure is fabricated by coating amorphous TiO2 on nanoporous BiVO4 with the aid of atomic layer deposition and further hydrogen plasma treatment at room temperature. The black BiVO4 with moderate oxygen vacancies reveals a bandgap reduction of ≈0.3 eV and significantly enhances solar utilization, charge transport and separation simultaneously, compared with conventional BiVO4. The amorphous layer of TiO2?x acts as both oxygen‐evolution catalyst and protection layer, which suppresses anodic photocorrosion to stabilize black BiVO4. This configuration of black BiVO4@amorphous TiO2?x may provide an effective strategy to prompt solar water splitting toward practical applications.  相似文献   

19.
For practical use of perovskite solar cells (PSCs) the instability issues of devices, attributed to degradation of perovskite molecules by moisture, ions migration, and thermal‐ and light‐instability, have to be solved. Herein, highly efficient and stable PSCs based on perovskite/Ag‐reduced graphene oxide (Ag‐rGO) and mesoporous Al2O3/graphene (mp‐AG) composites are reported. The mp‐AG composite is conductive with one‐order of magnitude higher mobility than mp‐TiO2 and used for electron transport layer (ETL). Compared to the mp‐TiO2 ETL based cells, the champion device based on perovskite/Ag‐rGO and SrTiO3/mp‐AG composites shows overall a best performance (i.e., VOC = 1.057 V, JSC = 25.75 mA cm?2, fill factor (FF) = 75.63%, and power conversion efficiency (PCE) = 20.58%). More importantly, the champion device without encapsulation exhibits not only remarkable thermal‐ and photostability but also long‐term stability, retaining 97–99% of the initial values of photovoltaic parameters and sustaining ≈93% of initial PCE over 300 d under ambient conditions.  相似文献   

20.
A novel scheme for hybridizing inkjet‐printed thin film Cu(In,Ga)Se2 (CIGS) solar cells with self‐assembled clusters of nanocrystal quantum dots (NQDs), which provides a 10.9% relative enhancement of the photon conversion efficiency (PCE), is demonstrated. A non‐uniform layer of NQD aggregates is deposited between the transparent conductive oxide and a CdS/CIGS p‐n junction using low cost pulsed‐spray deposition. Hybridization significantly improves the external quantum efficiency of the hybrid devices in the absorption range of the NQDs and in the red to near‐IR parts of the spectrum. The low wavelength response enhancement is found to be induced by luminescent down‐shifting (LDS) from the NQD layer, while the increase at longer wavelengths is attributed to internal scattering from NQD aggregates. LDS is demonstrated using time‐resolved spectroscopy, and the morphology of the NQD layer is investigated in fluorescence microscopy and cross‐sectional transmission electron microscopy. The influence of the NQD dose on the PCE of the hybrid devices is investigated and an optimum value is obtained. The low costs and limited material consumptions associated with pulsed‐spray deposition make these flexible hybrid devices promising candidates to help push thin‐film photovoltaic technology towards grid parity.  相似文献   

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