RESUMO
The interfacial electronic structure of perovskite layers and transport layers is critical for the performance and stability of perovskite solar cells (PSCs). The device performance of PSCs can generally be improved by adding a slight excess of lead iodide (PbI2 ) to the precursor solution. However, its underlying working mechanism is controversial. Here, we performed a comprehensive study of the electronic structures at the interface between CH3 NH3 PbI3 and C60 with and without the modification of PbI2 using inâ situ photoemission spectroscopy measurements. The correlation between the interfacial structures and the device performance was explored based on performance and stability tests. We found that there is an interfacial dipole reversal, and the downward band bending is larger at the CH3 NH3 PbI3 /C60 interface with the modification of PbI2 as compared to that without PbI2 . Therefore, PSCs with PbI2 modification exhibit faster charge carrier transport and slower carrier recombination. Nevertheless, the modification of PbI2 undermines the device stability due to aggravated iodide migration. Our findings provide a fundamental understanding of the CH3 NH3 PbI3 /C60 interfacial structure from the perspective of the atomic layer and insight into the double-edged sword effect of PbI2 as an additive.
RESUMO
Low-temperature solution-processed TiO2 nanocrystals (LT-TiO2) have been extensively applied as electron transport layer (ETL) of perovskite solar cells (PSCs). However, the low electron mobility, high density of electronic trap states, and considerable photocatalytic activity of TiO2 result in undesirable charge recombination at the ETL/perovskite interface and notorious instability of PSCs under ultraviolet (UV) light. Herein, LT-TiO2 nanocrystals are in situ fluorinated via a simple nonhydrolytic method, affording formation of TiâF bonds, and consequently increase electron mobility, decrease density of electronic trap states, and inhibit photocatalytic activity. Upon applying fluorinated TiO2 nanocrystals (F-TiO2) as ETL, regular-structure planar heterojunction PSC (PHJ-PSC) achieves a champion power conversion efficiency (PCE) of 22.68%, which is among the highest PCEs for PHJ-PSCs based on LT-TiO2 ETLs. Flexible PHJ-PSC devices based on F-TiO2 ETL exhibit the best PCE of 18.26%, which is the highest value for TiO2-based flexible devices. The bonded F atoms on the surface of TiO2 promote the formation of PbâF bonds and hydrogen bonds between F- and FA/MA organic cations, reinforcing interface binding of perovskite layer with TiO2 ETL. This contributes to effective passivation of the surface trap states of perovskite film, resulting in enhancements of device efficiency and stability especially under UV light.
RESUMO
Fullerene derivatives, especially [6,6]-phenyl-C61-butyric acid methyl ester (PCBM), have been widely applied as electron transport layers of inverted planar heterojunction perovskite solar cells (PSCs). However, the solution-processed PCBM capping layer suffers from limited surface wetting which hinders the improvement in efficiency and scalability of PSCs. Herein, we develop a facile hybrid solvent strategy that enables very fast wetting of the PCBM capping layer atop of the perovskite surface, leading to an improved interfacial contact and electron transport. The significantly enhanced wettability of the PCBM solution fulfilled through blending isopropyl alcohol into the commonly used chlorobenzene (CB) is attributed to the reduced surface tension while retaining viscosity. As a result, the electron mobility and electric conductivity of the PCBM capping layer increase by around two times, and the PSC devices exhibit the highest power conversion efficiency (PCE) of 19.92%, which is improved by â¼18% relative to that of the control device (16.78%). Importantly, this strategy is also applicable for other alcohols (ethanol and methanol) and CB blends. Moreover, the fast wetting approach enables us to deposit the PCBM capping layer using a facile drop-casting method, affording comparable PCEs to those obtained by the conventional spin-coating method, which is not achievable by using the conventional single solvent. This fast wetting PCBM capping layer also contributes to efficiency improvement of large-area (1 cm2) devices. These advances hold great potential for other scalable deposition methods such as blade-coating and slot-die coating.
RESUMO
An efficient one-pot three-component domino coupling reaction of phenols, C60, and bromoalkanes was developed, resulting in the highly regioselective synthesis of 1,4-asymmetrical C60 bisadducts. The reaction utilizes KOtBu as a promoter and likely proceeds by an oxyanion/carbanion rearrangement/nucleophilic addition cascade. This new methodology is particularly effective for the synthesis of 1,4-asymmetrical C60 electron transport materials. Its utility is demonstrated by the synthesis of a new efficient 1,4-C60 ETM, which possesses better performance, easier synthesis, and a lower cost compared with the commercially available PCBM.