skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Engineering ligand reactivity enables high-temperature operation of stable perovskite solar cells
Perovskite solar cells (PSCs) consisting of interfacial two- and three-dimensional heterostructures that incorporate ammonium ligand intercalation have enabled rapid progress toward the goal of uniting performance with stability. However, as the field continues to seek ever-higher durability, additional tools that avoid progressive ligand intercalation are needed to minimize degradation at high temperatures. We used ammonium ligands that are nonreactive with the bulk of perovskites and investigated a library that varies ligand molecular structure systematically. We found that fluorinated aniliniums offer interfacial passivation and simultaneously minimize reactivity with perovskites. Using this approach, we report a certified quasi–steady-state power-conversion efficiency of 24.09% for inverted-structure PSCs. In an encapsulated device operating at 85°C and 50% relative humidity, we document a 1560-hourT85at maximum power point under 1-sun illumination.  more » « less
Award ID(s):
1936527
PAR ID:
10491520
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more » ; ; ; ; ; ; « less
Publisher / Repository:
AAAS
Date Published:
Journal Name:
Science
Volume:
381
Issue:
6654
ISSN:
0036-8075
Page Range / eLocation ID:
209 to 215
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract The combined effects of compact TiO2(c‐TiO2) electron‐transport layer (ETL) are investigated without and with mesoscopic TiO2(m‐TiO2) on top, and without and with an iodine‐terminated silane self‐assembled monolayer (SAM), on the mechanical behavior, opto–electronic properties, photovoltaic (PV) performance, and operational‐stability of solar cells based on metal‐halide perovskites (MHPs). The interfacial toughness increases almost threefold in going from c‐TiO2without SAM to m‐TiO2with SAM. This is attributed to the synergistic effect of the m‐TiO2/MHP nanocomposite at the interface and the enhanced adhesion afforded by the iodine‐terminated silane SAM. The combination of m‐TiO2and SAM also offers a significant beneficial effect on the photocarriers extraction at the ETL/MHP interface, resulting in perovskite solar cells (PSCs) with power‐conversion efficiency (PCE) of over 24% and 20% for 0.1 and 1 cm2active areas, respectively. These PSCs also have exceptionally long operational‐stability lives: extrapolatedT80 (duration at 80% initial PCE retained) is ≈18 000 and 10 000 h for 0.1 and 1 cm2active areas, respectively.Postmortemcharacterization and analyses of the operational‐stability‐tested PSCs are performed to elucidate the possible mechanisms responsible for the long operational‐stability. 
    more » « less
  2. Mechanical failure and chemical degradation of device heterointerfaces can strongly influence the long-term stability of perovskite solar cells (PSCs) under thermal cycling and damp heat conditions. We report chirality-mediated interfaces based onR-/S-methylbenzyl-ammonium between the perovskite absorber and electron-transport layer to create an elastic yet strong heterointerface with increased mechanical reliability. This interface harnesses enantiomer-controlled entropy to enhance tolerance to thermal cycling–induced fatigue and material degradation, and a heterochiral arrangement of organic cations leads to closer packing of benzene rings, which enhances chemical stability and charge transfer. The encapsulated PSCs showed retentions of 92% of power-conversion efficiency under a thermal cycling test (−40°C to 85°C; 200 cycles over 1200 hours) and 92% under a damp heat test (85% relative humidity; 85°C; 600 hours). 
    more » « less
  3. Abstract 2D perovskites are recently attracting a significant amount of attention, mainly due to their improved stability compared with their 3D counterpart, e.g., the archetypical MAPbI3. Interestingly, the first studies on 2D perovskites can be dated back to the 1980s. The most popular 2D perovskites have a general formula of (RNH3)2MAn−1MnX3n+1, wherenrepresents the number of metal halide octahedrons between the insulating organic cation layers. The optoelectronic properties of 2D perovskites, e.g., band gap, are highly dependent on the thickness of the inorganic layers (i.e., the value ofn). Herein, 2D perovskites are arbitrarily divided into three classes, strict 2D (n= 1), quasi‐2D (n= 2–5), and quasi‐3D (n> 5), and research progress is summarized following this classification. The majority of existing 2D perovskites only employ very simple organic cations (e.g., butyl ammonium or phenylethyl ammonium), which merely function as the supporting layer/insulating barrier to achieve the 2D structure. Thus, a particularly important research question is: can functional organic cations be designed for these 2D perovskites, where these functional organic cations would play an important role in dictating the optoelectronic properties of these organic–inorganic hybrid materials, leading to unique device performance or applications? 
    more » « less
  4. Abstract State‐of‐the‐art perovskite solar cells (PSCs) have bandgaps that are invariably larger than 1.45 eV, which limits their theoretically attainable power conversion efficiency. The emergent mixed‐(Pb, Sn) perovskites with bandgaps of 1.2–1.3 eV are ideal for single‐junction solar cells according to the Shockley–Queisser limit, and they have the potential to deliver higher efficiency. Nevertheless, the high chemical activity of Sn(II) in these perovskites makes it extremely challenging to control their physical properties and chemical stability, thereby leading to PSCs with relatively low PCE and stability. In this work, the authors employ the Lewis‐adduct SnF2·3FACl additive in the solution‐processing of ideal‐bandgap halide perovskites (IBHPs), and prepare uniform large‐grain perovskite thin films containing continuously functionalized grain boundaries with the stable SnF2phase. Such Sn(II)‐rich grain‐boundary networks significantly enhance the physical properties and chemical stability of the IBHP thin films. Based on this approach, PSCs with an ideal bandgap of 1.3 eV are fabricated with a promising efficiency of 15.8%, as well as enhanced stability. The concept of Lewis‐adduct‐mediated grain‐boundary functionalization in IBHPs presented here points to a new chemical route for approaching the Shockley–Queisser limit in future stable PSCs. 
    more » « less
  5. Although C60is usually the electron transport layer (ETL) in inverted perovskite solar cells, its molecular nature of C60leads to weak interfaces that lead to non-ideal interfacial electronic and mechanical degradation. Here, we synthesized an ionic salt from C60, 4-(1',5′-dihydro-1'-methyl-2'H-[5,6] fullereno-C60-Ih-[1,9-c]pyrrol-2'-yl) phenylmethanaminium chloride (CPMAC), and used it as the electron shuttle in inverted PSCs. The CH2-NH3+head group in the CPMA cation improved the ETL interface and the ionic nature enhanced the packing, leading to ~3-fold increase in the interfacial toughness compared to C60. Using CPMAC, we obtained ~26% power conversion efficiencies (PCEs) with ~2% degradation after 2,100 hours of 1-sun operation at 65°C. For minimodules (four subcells, 6 centimeters square), we achieved the PCE of ~23% with <9% degradation after 2,200 hours of operation at 55°C. 
    more » « less