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1.
Adv Mater ; 34(50): e2206717, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36189867

RESUMEN

In contrast to classical bulk heterojunction (BHJ) in organic solar cells (OSCs), the quasi-homojunction (QHJ) with extremely low donor content (≤10 wt.%) is unusual and generally yields much lower device efficiency. Here, representative polymer donors and nonfullerene acceptors are selected to fabricate QHJ OSCs, and a complete picture for the operation mechanisms of high-efficiency QHJ devices is illustrated. PTB7-Th:Y6 QHJ devices at donor:acceptor (D:A) ratios of 1:8 or 1:20 can achieve 95% or 64% of the efficiency obtained from its BHJ counterpart at the optimal D:A ratio of 1:1.2, respectively, whereas QHJ devices with other donors or acceptors suffer from rapid roll-off of efficiency when the donors are diluted. Through device physics and photophysics analyses, it is observed that a large portion of free charges can be intrinsically generated in the neat Y6 domains rather than at the D/A interface. Y6 also serves as an ambipolar transport channel, so that hole transport as also mainly through Y6 phase. The key role of PTB7-Th is primarily to reduce charge recombination, likely assisted by enhancing quadrupolar fields within Y6 itself, rather than the previously thought principal roles of light absorption, exciton splitting, and hole transport.

2.
Adv Mater ; 34(42): e2205926, 2022 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-36027579

RESUMEN

Efficient exciton diffusion and charge transport play a vital role in advancing the power conversion efficiency (PCE) of organic solar cells (OSCs). Here, a facile strategy is presented to simultaneously enhance exciton/charge transport of the widely studied PM6:Y6-based OSCs by employing highly emissive trans-bis(dimesitylboron)stilbene (BBS) as a solid additive. BBS transforms the emissive sites from a more H-type aggregate into a more J-type aggregate, which benefits the resonance energy transfer for PM6 exciton diffusion and energy transfer from PM6 to Y6. Transient gated photoluminescence spectroscopy measurements indicate that addition of BBS improves the exciton diffusion coefficient of PM6 and the dissociation of PM6 excitons in the PM6:Y6:BBS film. Transient absorption spectroscopy measurements confirm faster charge generation in PM6:Y6:BBS. Moreover, BBS helps improve Y6 crystallization, and current-sensing atomic force microscopy characterization reveals an improved charge-carrier diffusion length in PM6:Y6:BBS. Owing to the enhanced exciton diffusion, exciton dissociation, charge generation, and charge transport, as well as reduced charge recombination and energy loss, a higher PCE of 17.6% with simultaneously improved open-circuit voltage, short-circuit current density, and fill factor is achieved for the PM6:Y6:BBS devices compared to the devices without BBS (16.2%).

3.
ACS Appl Energy Mater ; 5(8): 9351-9360, 2022 Aug 22.
Artículo en Inglés | MEDLINE | ID: mdl-36034762

RESUMEN

The goal of this work is to substitute the conventional high-cost poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) in inverted perovskite solar cells (PSCs) with an efficient and conducting polyaniline (PANI) polymer. The reported use of PANI in PSCs involves a chemical synthesis method which is prone to contamination with impurities as it requires several materials for polymerization and adhesion improvement with substrates, contributing to low device efficiencies. This work mitigates this issue using an electrochemical method that is low cost, less time consuming, and capable of producing thin films of PANI with excellent adhesion to substrates. Results demonstrated that the power conversion efficiency of the electrochemically synthesized PANI-based PSC is 16.94% versus 15.11% for the PEDOT:PSS-based device. It was observed that the work function of PANI was lower compared to that of PEDOT:PSS which decreased V OC but enhanced hole extraction at the hole transport layer/perovskite interface, thus increasing J SC. Doping electrolyte solution with lithium bis(trifluoromethanesulfonyl)imide LiTFSI increased the work function of PANI, thus increasing V OC from 0.87 to 0.93 V. This method enables simple and scalable synthesis of PANI as a competitive hole transport material to replace rather expensive PEDOT:PSS, thus enabling an important step toward low-cost inverted perovskite photovoltaic devices.

4.
Artículo en Inglés | MEDLINE | ID: mdl-35831209

RESUMEN

The combination of organic ligands and inorganic Pb-I frameworks in layered perovskites has bestowed upon them high structural tunability and stability, while their microscopic degradation mechanism remains unclear. Here, we found the key role of ligands in intrinsic structural stability and the consequent morphological evolution in layered perovskites during long-term ambient aging based on (GA)(MA)nPbnI3n+1 (GA = guanidinium, = 4) and (BDA)(MA)n-1PbnI3n+1 (BDA = 1,4-butanediammonium, < n > = 4) perovskites. The BDA-based perovskites have a low intrinsic stability due to high crystal formation energy (ΔH), which are prone to hydration during ambient aging. We overserved changed crystal orientation from perpendicular to parallel, a delayed charge populating time from <1 ps to >50 ps, an inhibited carrier transfer kinetics between quantum wells, an increase of 0.9 µs of charge carrier transport time and a decrease of 1.2 µs of charge carrier lifetime in the BDA-based film during ambient aging, which accounts for a large power-conversion efficiency (PCE) loss (14.2% vs 11.2%). By contrast, the GA ligand increases the intrinsic structural stability of perovskites, which not only yields an initial PCE as high as 20.0% but also helps retain excellent optoelectronic properties during aging. Therefore, only a slight PCE loss (20.0% vs 19.1%) was observed. Our work reveals the key role of organic-inorganic interaction affecting the intrinsic structural stability and optoelectronic properties, and provides a theoretical basis for the future design of stable and efficient optoelectronic devices.

5.
ACS Appl Energy Mater ; 5(1): 648-657, 2022 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-35098044

RESUMEN

Solid-state lithium batteries are generally considered as the next-generation battery technology that benefits from inherent nonflammable solid electrolytes and safe harnessing of high-capacity lithium metal. Among various solid-electrolyte candidates, cubic garnet-type Li7La3Zr2O12 ceramics hold superiority due to their high ionic conductivity (10-3 to 10-4 S cm-1) and good chemical stability against lithium metal. However, practical deployment of solid-state batteries based on such garnet-type materials has been constrained by poor interfacing between lithium and garnet that displays high impedance and uneven current distribution. Herein, we propose a facile and effective strategy to significantly reduce this interfacial mismatch by modifying the surface of such garnet-type solid electrolyte with a thin layer of silicon nitride (Si3N4). This interfacial layer ensures an intimate contact with lithium due to its lithiophilic nature and formation of an intermediate lithium-metal alloy. The interfacial resistance experiences an exponential drop from 1197 to 84.5 Ω cm2. Lithium symmetrical cells with Si3N4-modified garnet exhibited low overpotential and long-term stable plating/stripping cycles at room temperature compared to bare garnet. Furthermore, a hybrid solid-state battery with Si3N4-modified garnet sandwiched between lithium metal anode and LiFePO4 cathode was demonstrated to operate with high cycling efficiency, excellent rate capability, and good electrochemical stability. This work represents a significant advancement toward use of garnet solid electrolytes in lithium metal batteries for the next-generation energy storage devices.

6.
ACS Appl Mater Interfaces ; 12(37): 41312-41322, 2020 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-32829634

RESUMEN

Perovskites have been unprecedented with a relatively sharp rise in power conversion efficiency in the last decade. However, the polycrystalline nature of the perovskite film makes it susceptible to surface and grain boundary defects, which significantly impedes its potential performance. Passivation of these defects has been an effective approach to further improve the photovoltaic performance of the perovskite solar cells. Here, we report the use of a novel hydrazine-based aromatic iodide salt or phenyl hydrazinium iodide (PHI) for secondary post treatment to passivate surface and grain boundary defects in triple cation mixed halide perovskite films. In particular, the PHI post treatment reduced current at the grain boundaries, facilitated an electron barrier, and reduced trap state density, indicating suppression of leakage pathways and charge recombination, thus passivating the grain boundaries. As a result, a significant enhancement in power conversion efficiency to 20.6% was obtained for the PHI-treated perovskite device in comparison to a control device with 17.4%.

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