skip to main content


Title: Fusing Nanowires into Thin Films: Fabrication of Graded‐Heterojunction Perovskite Solar Cells with Enhanced Performance
Abstract

Perovskite solar cells (PSCs) have recently experienced a rapid rise in power conversion efficiency (PCE), but the prevailing PSCs with conventional mesoscopic or planar device architectures still contain nonideal perovskite/hole‐transporting‐layer (HTL) interfaces, limiting further enhancement in PCE and device stability. In this work, CsPbBr3perovskite nanowires are employed for modifying the surface electronic states of bulk perovskite thin films, forming compositionally‐graded heterojunction at the perovskite/HTL interface of PSCs. The nanowire morphology is found to be key to achieving lateral homogeneity in the perovskite film surface states resulting in a near‐ideal graded heterojunction. The hidden role of such lateral homogeneity on the performance of graded‐heterojunction PSCs is revealed for the first time. The resulting PSCs show high PCE up to 21.4%, as well as high operational stability, which is superior to control PSCs fabricated without CsPbBr3‐nanocrystals modification and with CsPbBr3‐nanocubes modification. This study demonstrates the promise of controlled hybridization of perovskite nanowires and bulk thin films for more efficient and stable PSCs.

 
more » « less
NSF-PAR ID:
10461210
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Energy Materials
Volume:
9
Issue:
22
ISSN:
1614-6832
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Flexible perovskite solar cells (f‐PSCs) have attracted great attention due to their promising commercial prospects. However, the performance off‐PSCs is generally worse than that of their rigid counterparts. Herein, it is found that the unsatisfactory performance of planar heterojunction (PHJ)f‐PSCs can be attributed to the undesirable morphology of electron transport layer (ETL), which results from the rough surface of the flexible substrate. Precise control over the thickness and morphology of ETL tin dioxide (SnO2) not only reduces the reflectance of the indium tin oxide (ITO) on polyethylene 2,6‐naphthalate (PEN) substrate and enhances photon collection, but also decreases the trap‐state densities of perovskite films and the charge transfer resistance, leading to a great enhancement of device performance. Consequently, thef‐PSCs, with a structure of PEN/ITO/SnO2/perovskite/Spiro‐OMeTAD/Ag, exhibit a power conversion efficiency (PCE) up to 19.51% and a steady output of 19.01%. Furthermore, thef‐PSCs show a robust bending resistance and maintain about 95% of initial PCE after 6000 bending cycles at a bending radius of 8 mm, and they present an outstanding long‐term stability and retain about 90% of the initial performance after >1000 h storage in air (10% relative humidity) without encapsulation.

     
    more » « less
  2. Abstract

    The presence of surface and grain boundary defects in organic–inorganic halide perovskite films can be detrimental to both the performance and operational stability of perovskite solar cells (PSCs). Here, the effect of chloride additives is studied on the bulk and surface defects of the mixed cation and halide PSCs. It is found that using an antisolvent technique, the perovskite film is divided into two layers, i.e., a bottom layer with large grains and a thin capping layer with small grains. The addition of formamidinium chloride (FACl) into the precursor solution removes the small‐grained perovskite capping layer and suppresses the formation of bulk and surface defects, providing a perovskite film with enhanced crystallinity and large grain size of over 1 µm. Time‐resolved photoluminescence measurements show longer lifetimes for perovskite films modified by FACl and subsequently passivated by 1‐adamantylamine hydrochloride as compared to the reference sample. Impedance spectroscopy measurements show that these treatments reduce the recombination in the PSCs, leading to a champion device with power conversion efficiency (PCE) of 21.2%, an open circuit voltage of 1152 mV and negligible hysteresis. The Cl treated PSC also shows improved operational stability with only 12% PCE loss after 700 h under continuous illumination.

     
    more » « less
  3. Abstract

    Surface passivation of perovskite solar cells (PSCs) using a low‐cost industrial organic pigment quinacridone (QA) is presented. The procedure involves solution processing a soluble derivative of QA,N,N‐bis(tert‐butyloxycarbonyl)‐quinacridone (TBOC‐QA), followed by thermal annealing to convert TBOC‐QA into insoluble QA. With halide perovskite thin films coated by QA, PSCs based on methylammonium lead iodide (MAPbI3) showed significantly improved performance with remarkable stability. A PCE of 21.1 % was achieved, which is much higher than 18.9 % recorded for the unmodified devices. The QA coating with exceptional insolubility and hydrophobicity also led to greatly enhanced contact angle from 35.6° for the pristine MAPbI3thin films to 77.2° for QA coated MAPbI3thin films. The stability of QA passivated MAPbI3perovskite thin films and PSCs were significantly enhanced, retaining about 90 % of the initial efficiencies after more than 1000 hours storage under ambient conditions.

     
    more » « less
  4. Abstract

    Surface passivation of perovskite solar cells (PSCs) using a low‐cost industrial organic pigment quinacridone (QA) is presented. The procedure involves solution processing a soluble derivative of QA,N,N‐bis(tert‐butyloxycarbonyl)‐quinacridone (TBOC‐QA), followed by thermal annealing to convert TBOC‐QA into insoluble QA. With halide perovskite thin films coated by QA, PSCs based on methylammonium lead iodide (MAPbI3) showed significantly improved performance with remarkable stability. A PCE of 21.1 % was achieved, which is much higher than 18.9 % recorded for the unmodified devices. The QA coating with exceptional insolubility and hydrophobicity also led to greatly enhanced contact angle from 35.6° for the pristine MAPbI3thin films to 77.2° for QA coated MAPbI3thin films. The stability of QA passivated MAPbI3perovskite thin films and PSCs were significantly enhanced, retaining about 90 % of the initial efficiencies after more than 1000 hours storage under ambient conditions.

     
    more » « less
  5. Abstract

    Two key interfaces in flexible perovskite solar cells (f‐PSCs) are mechanically reinforced simultaneously: one between the electron‐transport layer (ETL) and the 3D metal‐halide perovskite (MHP) thin film using self‐assembled monolayer (SAM), and the other between the 3D‐MHP thin film and the hole‐transport layer (HTL) using an in situ grown low‐dimensional (LD) MHP capping layer. The interfacial mechanical properties are measured and modeled. This rational interface engineering results in the enhancement of not only the mechanical properties of both interfaces but also their optoelectronic properties holistically. As a result, the new class of dual‐interface‐reinforced f‐PSCs has an unprecedented combination of the following three important performance parameters: high power‐conversion efficiency (PCE) of 21.03% (with reduced hysteresis), improved operational stability of 1000 hT90(duration at 90% initial PCE retained), and enhanced mechanical reliability of 10 000 cyclesn88(number of bending cycles at 88% initial PCE retained). The scientific underpinnings of these synergistic enhancements are elucidated.

     
    more » « less