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1.
An efficient electron transport layer (ETL) plays a key role in promoting carrier separation and electron extraction in planar perovskite solar cells (PSCs). An effective composite ETL is fabricated using carboxylic-acid- and hydroxyl-rich red-carbon quantum dots (RCQs) to dope low-temperature solution-processed SnO2, which dramatically increases its electron mobility by ≈20 times from 9.32 × 10−4 to 1.73 × 10−2 cm2 V−1 s−1. The mobility achieved is one of the highest reported electron mobilities for modified SnO2. Fabricated planar PSCs based on this novel SnO2 ETL demonstrate an outstanding improvement in efficiency from 19.15% for PSCs without RCQs up to 22.77% and have enhanced long-term stability against humidity, preserving over 95% of the initial efficiency after 1000 h under 40–60% humidity at 25 °C. These significant achievements are solely attributed to the excellent electron mobility of the novel ETL, which is also proven to help the passivation of traps/defects at the ETL/perovskite interface and to promote the formation of highly crystallized perovskite, with an enhanced phase purity and uniformity over a large area. These results demonstrate that inexpensive RCQs are simple but excellent additives for producing efficient ETLs in stable high-performance PSCs as well as other perovskite-based optoelectronics.  相似文献   

2.
In planar perovskite solar cells, it is vital to engineer the extraction and recombination of electron–hole pairs at the electron transport layer/perovskite interface for obtaining high performance. This study reports a novel titanium oxide (TiO2) bilayer with different Fermi energy levels by combing atomic layer deposition and spin‐coating technique. Energy band alignments of TiO2 bilayer can be modulated by controlling the deposition order of layers. The TiO2 bilayer based perovskite solar cells are highly efficient in carrier extraction, recombination suppression, and defect passivation, and thus demonstrate champion efficiencies up to 16.5%, presenting almost 50% enhancement compared to the TiO2 single layer based counterparts. The results suggest that the bilayer with type II band alignment as electron transport layers provides an efficient approach for constructing high‐performance planar perovskite solar cells.  相似文献   

3.

In the conventional perovskite solar cells (PSCs) structure, TiO2 is the most commonly used electron transport layer (ETL) as it has good energy-level matching with perovskite layer. However, oxygen vacancy defects will appear when TiO2 is exposed to ultraviolet light for a long time, which would reduce its carrier extraction ability. Here, we report a simple and effective interface engineering method for TiO2 ETL to achieve a highly efficient PSCs. An ultra-thin [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) layer is used to modify the mesoporous TiO2/perovskite layer interface. The PCBM effectively passivates defects on the TiO2 surface, promotes the extraction of electrons, and improves the quality of the perovskite film. Finally, a high efficiency of 16.4% was achieved for the modified device, much higher than 13.5% of the reference devices. After storing for 12 days in an atmosphere with an air humidity of 30?±?5%, the efficiency of the PSCs maintains more than 60% of its initial level. This strategy is beneficial to enhance the efficiency and working stability of PSCs.

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4.
Ordered 1D metal oxide structure is desirable in thin film solar cells owing to its excellent charge collection capability. However, the electron transfer in 1D electron transporting layer (ETL)‐based devices is still limited to a submicrometer‐long pathway that is vertical to the substrate. Here, an innovative closely packed rutile TiO2 nanowire (CRTNW) network parallel to the facet of fluorine‐doped tin oxide (FTO) substrate is reported, which can serve as a 1D nanoscale electron transport pathway for efficient perovskite solar cells (PSCs). The PSC constructed using newly prepared CRTNW ETL achieves an impressive power conversion efficiency of 21.10%, which can be attributed to the facilitated electron extraction induced by the favorable junctions formed at FTO/ETL and ETL/perovskite interfaces and also the suppressed charge recombination originating from improved perovskite morphology with large grains, flat surface, and good surface coverage. The bifacial contact junctions engineering also enables large‐area device fabrication. The PSC with 1 cm2 aperture yields an efficiency of 19.50% under one sun illumination. This work highlights the significance of controlling the orientation and packing density of the ordered 1D oxide nanostructured thin films for highly efficient optoelectronic devices in a large‐scale manner.  相似文献   

5.
Nanostructured tin (IV) oxide (SnO2) is emerging as an ideal inorganic electron transport layer in n–i–p perovskite devices, due to superior electronic and low‐temperature processing properties. However, significant differences in current–voltage performance and hysteresis phenomena arise as a result of the chosen fabrication technique. This indicates enormous scope to optimize the electron transport layer (ETL), however, to date the understanding of the origin of these phenomena is lacking. Reported here is a first comparison of two common SnO2 ETLs with contrasting performance and hysteresis phenomena, with an experimental strategy to combine the beneficial properties in a bilayer ETL architecture. In doing so, this is demonstrated to eliminate room‐temperature hysteresis while simultaneously attaining impressive power conversion efficiency (PCE) greater than 20%. This approach highlights a new way to design custom ETLs using functional thin‐film coatings of nanomaterials with optimized characteristics for stable, efficient, perovskite solar cells.  相似文献   

6.
Titanium oxide (TiO2) has been widely used as an electron transport layer (ETL) in perovskite solar cells (PSCs). Typically, TiCl4 post-treatment is indispensable for modifying the surfaces of TiO2 ETL to improve the electron transport performance. However, it is challenging to produce the preferred anatase phase-dominated TiO2 by the TiCl4 post-treatment due to the higher thermodynamic stability of the rutile phase. In this work, a mild continuous pH control strategy for effectively regulating the hydrolysis process of TiCl4 post-treatment is proposed. As the weak organic base, urea has been demonstrated can maintain a moderate pH decrease during the hydrolysis process of TiCl4 while keeping the hydrolysis process relatively mild due to the ultra-weak alkalinity. The improved pH environment is beneficial for the formation of anatase TiO2. Consequently, a uniform anatase-dominated TiO2 surface layer is formed on the mesoporous TiO2, resulting in reduced defect density and superior band energy level. The interfacial charge recombination is effectively suppressed, and the charge extraction efficiency is improved simultaneously in the fabricated solar cells. The efficiency of the fabricated carbon electrode-based PSCs (C-PSCs) is improved from 16.63% to 18.08%, which is the highest for C-PSCs based on wide-bandgap perovskites.  相似文献   

7.
The low electrical conductivity and the high surface defect density of the TiO2 electron transport layer (ETL) limit the power conversion efficiency (PCE) of corresponding perovskite solar cells (PSCs). Here, the conductivity and defect modulation of the mesoporous TiO2 (mp-TiO2) ETL via oxygen vacancy (OV) management by the reduction and oxidation treatment are reported. Reduction treatment via reducing agent introduces abundant OVs into the TiO2 nanocrystalline particles on the surface and at the subsurface. The following oxidation treatment via hydrogen peroxide removes the surface OVs while remains the subsurface OVs, resulting in stratified OVs. The stratified OVs improve the conductivity of TiO2 ETL by increasing carrier donors and decrease nonradiative centers by reducing surface defects. Such synergy ensures the capability of mp-TiO2 as the well-performed ETL with improved energy level alignment, suppressed interface recombination, enhanced carrier extraction, and transport. As a result, printable hole-conductor-free carbon-based mesoscopic PSCs based on the modulated mp-TiO2 ETL demonstrate a highest reported PCE of 18.96%.  相似文献   

8.
Perovskite solar cells (PSCs) based on the SnO2 electron transport layer (ETL) have achieved remarkable photovoltaic efficiency. However, the commercial SnO2 ETLs show various shortcomings. The SnO2 precursor is prone to agglomeration, resulting in poor morphology with numerous interface defects. Additionally, the open circuit voltage (Voc) would be constrained by the energy level mismatch between the SnO2 and the perovskite. And, few studies designed SnO2-based ETLs to promote crystal growth of PbI2, a crucial prerequisite for obtaining high-quality perovskite films via the two-step method. Herein, we proposed a novel bilayer SnO2 structure that combined the atomic layer deposition (ALD) and sol-gel solution to well address the aforementioned issues. Due to the unique conformal effect of ALD-SnO2, it can effectively modulate the roughness of FTO substrate, enhance the quality of ETL, and induce the growth of PbI2 crystal phase to develop the crystallinity of perovskite layer. Furthermore, a created built-in field of the bilayer SnO2 can help to overcome the electron accumulation at the ETL/perovskite interface, leading to a higher Voc and fill factor. Consequently, the efficiency of PSCs with ionic liquid solvent increases from 22.09% to 23.86%, maintaining 85% initial efficiency in a 20% humidity N2 environment for 1300 h.  相似文献   

9.

Carbon-based perovskite solar cells (C-PSCs) have been popular for achieving low-cost and stable photovoltaics. To overcome an obstacle of high-temperature annealing process for producing titanium dioxide (TiO2), CsPbI2Br C-PSCs based on a device structure of FTO/tin oxide (SnO2)/CsPbI2Br/carbon electrode can be fabricated at the low-temperature annealing process of 280 °C for 180 s, where SnO2 is used as the electron transporting layer (ETL). Experimental results showed that the suitable concentration of SnO2 ETL could yield smooth surface CsPbI2Br films with free-pinhole and larger grain-sized crystallization. In combination with prolonging annealing time, a champion power conversion efficiency of 9.68% with a larger open-circuit voltage (Voc) of 1.14 V was obtained for CsPbI2Br C-PSC based on SnO2 ETL. Here, a simple low-temperature fabricating process of SnO2 ETL can be adapted to flexible substrates for C-PSCs and furtherly reduce the manufacturing cost.

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10.
In this work, a SnO2/ZnO bilayered electron transporting layer (ETL) aimed to achieve low energy loss and large open‐circuit voltage (Voc) for high‐efficiency all‐inorganic CsPbI2Br perovskite solar cells (PVSCs) is introduced. The high‐quality CsPbI2Br film with regular crystal grains and full coverage can be realized on the SnO2/ZnO surface. The higher‐lying conduction band minimum of ZnO facilitates desirable cascade energy level alignment between the perovskite and SnO2/ZnO bilayered ETL with superior electron extraction capability, resulting in a suppressed interfacial trap‐assisted recombination with lower charge recombination rate and greater charge extraction efficiency. The as‐optimized all‐inorganic PVSC delivers a high Voc of 1.23 V and power conversion efficiency (PCE) of 14.6%, which is one of the best efficiencies reported for the Cs‐based all‐inorganic PVSCs to date. More importantly, decent thermal stability with only 20% PCE loss is demonstrated for the SnO2/ZnO‐based CsPbI2Br PVSCs after being heated at 85 °C for 300 h. These findings provide important interface design insights that will be crucial to further improve the efficiency of all‐inorganic PVSCs in the future.  相似文献   

11.
Titanium oxide (TiO2) has been commonly used as an electron transport layer (ETL) of regular‐structure perovskite solar cells (PSCs), and so far the reported PSC devices with power conversion efficiencies (PCEs) over 21% are mostly based on mesoporous structures containing an indispensable mesoporous TiO2 layer. However, a high temperature annealing (over 450 °C) treatment is mandatory, which is incompatible with low‐cost fabrication and flexible devices. Herein, a facile one‐step, low‐temperature, nonhydrolytic approach to in situ synthesizing amino‐functionalized TiO2 nanoparticles (abbreviated as NH2‐TiO2 NPs) is developed by chemical bonding of amino (‐NH2) groups, via Ti? N bonds, onto the surface of TiO2 NPs. NH2‐TiO2 NPs are then incorporated as an efficient ETL in n‐i‐p planar heterojunction (PHJ) PSCs, affording PCE over 21%. Cs0.05FA0.83MA0.12PbI2.55Br0.45 (abbreviated as CsFAMA) PHJ PSC devices based on NH2‐TiO2 ETL exhibit the best PCE of 21.33%, which is significantly higher than that of the devices based on the pristine TiO2 ETL (19.82%) and is close to the record PCE for devices with similar structures and fabrication procedures. Besides, due to the passivation of the surface trap states of perovskite film, the hysteresis of current–voltage response is significantly suppressed, and the ambient stability of devices is improved upon amino functionalization.  相似文献   

12.
Carbon‐based perovskite solar cells (PVSCs) without hole transport materials are promising for their high stability and low cost, but the electron transporting layer (ETL) of TiO2 is notorious for inflicting hysteresis and instability. In view of its electron accepting ability, C60 is used to replace TiO2 for the ETL, forming a so‐called all carbon based PVSC. With a device structure of fluorine‐doped tin oxide (FTO)/C60/methylammonium lead iodide (MAPbI3)/carbon, a power conversion efficiency (PCE) is attained up to 15.38% without hysteresis, much higher than that of the TiO2 ones (12.06% with obvious hysteresis). The C60 ETL is found to effectively improve electron extraction, suppress charge recombination, and reduce the sub‐bandgap states at the interface with MAPbI3. Moreover, the all carbon based PVSCs are shown to resist moisture and ion migration, leading to a much higher operational stability under ambient, humid, and light‐soaking conditions. To make it an even more genuine all carbon based PVSC, it is further attempted to use graphene as the transparent conductive electrode, reaping a PCE of 13.93%. The high performance of all carbon based PVSCs stems from the bonding flexibility and electronic versatility of carbon, promising commercial developments on account of their favorable balance of cost, efficiency, and stability.  相似文献   

13.
An electron-transport layer (ETL) with appropriate energy alignment and enhanced charge transfer is critical for perovskite solar cells (PSCs). However, interfacial energy level mismatch limits the electrical performance of PSCs, particularly the open-circuit voltage (VOC). Herein, a simple low-temperature-processed In2O3/SnO2 bilayer ETL is developed and used for fabricating a new PSC device. The presence of In2O3 results in uniform, compact, and low-trap-density perovskite films. Moreover, the conduction band of In2O3 is shallower than that of Sn-doped In2O3 (ITO), enhancing the charge transfer from perovskite to ETL, thus minimizing VOC loss at the perovskite and ETL interface. A planar PSC with a power conversion efficiency of 23.24% (certified efficiency of 22.54%) is obtained. A high VOC of 1.17 V is achieved with the potential loss at only 0.36 V. In contrast, devices based on single SnO2 layers achieve 21.42% efficiency with a VOC of 1.13 V. In addition, the new device maintains 97.5% initial efficiency after 80 d in N2 without encapsulation and retains 91% of its initial efficiency after 180 h under 1 sun continuous illumination. The results demonstrate and pave the way for the development of efficient photovoltaic devices.  相似文献   

14.
Perovskite solar cells (PSCs) have rapidly developed and achieved power conversion efficiencies of over 20% with diverse technical routes. Particularly, planar-structured PSCs can be fabricated with low-temperature (≤150 °C) solution-based processes, which is energy efficient and compatible with flexible substrates. Here, the efficiency and stability of planar PSCs are enhanced by improving the interface contact between the SnO2 electron-transport layer (ETL) and the perovskite layer. A biological polymer (heparin potassium, HP) is introduced to regulate the arrangement of SnO2 nanocrystals, and induce vertically aligned crystal growth of perovskites on top. Correspondingly, SnO2–HP-based devices can demonstrate an average efficiency of 23.03% on rigid substrates with enhanced open-circuit voltage (VOC) of 1.162 V and high reproducibility. Attributed to the strengthened interface binding, the devices obtain high operational stability, retaining 97% of their initial performance (power conversion efficiency, PCE > 22%) after 1000 h operation at their maximum power point under 1 sun illumination. Besides, the HP-modified SnO2 ETL exhibits promising potential for application in flexible and large-area devices.  相似文献   

15.
Despite the rapid increase of efficiency, perovskite solar cells (PSCs) still face some challenges, one of which is the current–voltage hysteresis. Herein, it is reported that yttrium‐doped tin dioxide (Y‐SnO2) electron selective layer (ESL) synthesized by an in situ hydrothermal growth process at 95 °C can significantly reduce the hysteresis and improve the performance of PSCs. Comparison studies reveal two main effects of Y doping of SnO2 ESLs: (1) it promotes the formation of well‐aligned and more homogeneous distribution of SnO2 nanosheet arrays (NSAs), which allows better perovskite infiltration, better contacts of perovskite with SnO2 nanosheets, and improves electron transfer from perovskite to ESL; (2) it enlarges the band gap and upshifts the band energy levels, resulting in better energy level alignment with perovskite and reduced charge recombination at NSA/perovskite interfaces. As a result, PSCs using Y‐SnO2 NSA ESLs exhibit much less hysteresis and better performance compared with the cells using pristine SnO2 NSA ESLs. The champion cell using Y‐SnO2 NSA ESL achieves a photovoltaic conversion efficiency of 17.29% (16.97%) when measured under reverse (forward) voltage scanning and a steady‐state efficiency of 16.25%. The results suggest that low‐temperature hydrothermal‐synthesized Y‐SnO2 NSA is a promising ESL for fabricating efficient and hysteresis‐less PSC.  相似文献   

16.
In recent years, carbon-based CsPbI2Br perovskite solar cells (PSCs) have attracted more attention due to their low cost and good stability. However, the power conversion efficiency (PCE) of carbon-based CsPbI2Br PSCs is still no more than 16%, because of the defects in CsPbI2Br or at the interface with the electron transport layer (ETL), as well as the energy level mismatch, which lead to the loss of energy, thus limiting PCE values. Herein, a series of cadmium halides are introduced, including CdCl2, CdBr2 and CdI2 for dual direction thermal diffusion treatment. Some Cd2+ ions thermally diffuse downward to passivate the defects inside or on the surface of SnO2 ETL. Meanwhile, the energy level structure of SnO2 ETL is adjusted, which is in favor of the transfer of electron carriers and blocking holes. On the other hand, part of Cd2+ and Cl ions thermally diffuse upward into the CsPbI2Br lattice to passivate crystal defects. Through dual direction thermal diffusion treatment by CdCl2, CdI2 and CdBr2, the performance of devices has been significantly improved, and their PCE has been increased from 13.01% of the original device to 14.47%, 14.31%, and 13.46%, respectively. According to existing reports, 14.47% is one of the highest PCE of carbon-based CsPbI2Br PSCs with SnO2 ETLs.  相似文献   

17.
The interface engineering plays a key role in controlled optoelectronic properties of perovskite photovoltaic devices,and thus the electron transport layer(ETL) material with tailored optoelectronic properties remains a challenge for achieving high photovoltaic performance of planar perovskite solar cells(PSCs).Here,the fine and crystalline zirconium stanate(ZrSnO_4) nanoparticles(NPs) was synthesized at low temperature,and its optoelectronic properties are systematically investigated.Benefiting from the favorable electronic structure of ZrSnO_4 NPs for applications in ETL,efficient electron transport and extraction with suppre s sed charge recombination are achieved at the interface of perovskite layer.As a result,the optimized ZrSnO_4 NPs synthesized at room-temperature deliver the optimized power conversion efficiency up to 16.76% with acceptable stability.This work opens up a new class of ternary metal oxide for the use in ETL of the planar PSCs and should pave the way toward designing new interfacial materials for practical optoelectronic devices.  相似文献   

18.
In this study, the fabrication of highly efficient and durable flexible inverted perovskite solar cells (PSCs) is reported. Presynthesized, solution‐derived NiOx and ZnO nanoparticles films are employed at room temperature as a hole transport layer (HTL) and electron transport layer (ETL), respectively. The triple cation perovskite films are produced in a single step and for the sake of comparison, ultrasmooth and pinhole‐free absorbing layers are also fabricated using MAPbI3 perovskite. The triple cation perovskite cells exhibit champion power conversion efficiencies (PCEs) of 18.6% with high stabilized power conversion efficiency of 17.7% on rigid glass/indium tin oxide (ITO) substrates (comparing with 16.6% PCE with 16.1% stabilized output efficiency for the flexible polyethylene naphthalate (PEN)/thin film barrier/ITO substrates). More interestingly, the durability of flexible PSC under simulation of operative condition is proved. Over 85% of the maximum stabilized output efficiency is retained after 1000 h aging employing a thin MAPbI3 perovskite (over 90% after 500 h with a thick triple cation perovskite). This result is comparable to a similar state of the art rigid PSC and represents a breakthrough in the stability of flexible PSC using ETLs and HTLs compatible with roll to roll production speed, thanks to their room temperature processing.  相似文献   

19.
Corrosive precursors used for the preparation of organic–inorganic hybrid perovskite photoactive layers prevent the application of ultrathin metal layers as semitransparent bottom electrodes in perovskite solar cells (PVSCs). This study introduces tin‐oxide (SnOx) grown by atomic layer deposition (ALD), whose outstanding permeation barrier properties enable the design of an indium‐tin‐oxide (ITO)‐free semitransparent bottom electrode (SnOx/Ag or Cu/SnOx), in which the metal is efficiently protected against corrosion. Simultaneously, SnOx functions as an electron extraction layer. We unravel the spontaneous formation of a PbI2 interfacial layer between SnOx and the CH3NH3PbI3 perovskite. An interface dipole between SnOx and this PbI2 layer is found, which depends on the oxidant (water, ozone, or oxygen plasma) used for the ALD growth of SnOx. An electron extraction barrier between perovskite and PbI2 is identified, which is the lowest in devices based on SnOx grown with ozone. The resulting PVSCs are hysteresis‐free with a stable power conversion efficiency (PCE) of 15.3% and a remarkably high open circuit voltage of 1.17 V. The ITO‐free analogues still achieve a high PCE of 11%.  相似文献   

20.
The carrier concentration of the electron‐selective layer (ESL) and hole‐selective layer can significantly affect the performance of organic–inorganic lead halide perovskite solar cells (PSCs). Herein, a facile yet effective two‐step method, i.e., room‐temperature colloidal synthesis and low‐temperature removal of additive (thiourea), to control the carrier concentration of SnO2 quantum dot (QD) ESLs to achieve high‐performance PSCs is developed. By optimizing the electron density of SnO2 QD ESLs, a champion stabilized power output of 20.32% for the planar PSCs using triple cation perovskite absorber and 19.73% for those using CH3NH3PbI3 absorber is achieved. The superior uniformity of low‐temperature processed SnO2 QD ESLs also enables the fabrication of ≈19% efficiency PSCs with an aperture area of 1.0 cm2 and 16.97% efficiency flexible device. The results demonstrate the promise of carrier‐concentration‐controlled SnO2 QD ESLs for fabricating stable, efficient, reproducible, large‐scale, and flexible planar PSCs.  相似文献   

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