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1.
Adv Sci (Weinh) ; 11(17): e2307152, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38417119

RESUMEN

Dopant-free hole transport layers (HTLs) are crucial in enhancing perovskite solar cells (pero-SCs). Nevertheless, conventional processing of these HTL materials involves using toxic solvents, which gives rise to substantial environmental concerns and renders them unsuitable for large-scale industrial production. Consequently, there is a pressing need to develop dopant-free HTL materials processed using green solvents to facilitate the production of high-performance pero-SCs. Recently, several strategies have been developed to simultaneously improve the solubility of these materials and regulate molecular stacking for high hole mobility. In this review, a comprehensive overview of the methodologies utilized in developing dopant-free HTL materials processed from green solvents is provided. First, the study provides a brief overview of fundamental information about green solvents and Hansen solubility parameters, which can serve as a guideline for the molecular design of optimal HTL materials. Second, the intrinsic relationships between molecular structure, solubility in green solvents, molecular stacking, and device performance are discussed. Finally, conclusions and perspectives are presented along with the rational design of highly efficient, stable, and green solvent-processable dopant-free HTL materials.

2.
Angew Chem Int Ed Engl ; 62(46): e202312231, 2023 Nov 13.
Artículo en Inglés | MEDLINE | ID: mdl-37750462

RESUMEN

The use of dopant-free hole transport layers (HTLs) is critical in stabilizing n-i-p perovskite solar cells (pero-SCs). However, these HTL materials are often processed with toxic solvents, which is not ideal for industrial production. Upon substituting them with green solvents, a trade-off emerges between maintaining the high crystallinity of the HTL materials and ensuring high solubility in the new solvents. In this paper, we designed a novel, linear, organic small molecule, BDT-C8-3O, by introducing an asymmetric polar oligo(ethylene glycol) side chain. This method not only overcomes the solubility limitations in green solvents but also enables stacking the conjugated main chains in two patterns, which further enhances crystallinity and hole mobility. As a result, the n-i-p pero-SCs based on chlorobenzene- or green (natural compound) solvent 3-methylcyclohexanone-processed BDT-C8-3O HTL that without any dopant delivered world-recorded power conversion efficiencies of 24.11 % (certified of 23.82 %) and 23.53 %, respectively. The devices also demonstrated remarkable operational and high-temperature stabilities, maintaining over 84 % and 79.5 % of their initial efficiency for 2000 h, respectively. Encouragingly, dopant-free BDT-C8-3O HTL exhibits significant advantages in large-area fabrication, achieving state-of-the-art PCEs exceeding 20 % for 5×5 cm2 modules (active area: 15.64 cm2 ), even when processed using green solvents.

3.
Angew Chem Int Ed Engl ; 62(16): e202300690, 2023 Apr 11.
Artículo en Inglés | MEDLINE | ID: mdl-36811515

RESUMEN

The stability-related issues arising from the perovskite precursor inks, films, device structures and interdependence remain severely under-explored to date. Herein, we designed an ionic-liquid polymer (poly[Se-MI][BF4 ]), containing functional moieties like carbonyl (C=O), selenium (Se+ ), and tetrafluoroborate (BF4 - ) ions, to stabilize the whole device fabrication process. The C=O and Se+ can coordinate with lead and iodine (I- ) ions to stabilize lead polyhalide colloids and the compositions of the perovskite precursor inks for over two months. The Se+ anchored on grain boundaries and the defects passivated by BF4 - efficiently suppress the dissociation and migration of I- in perovskite films. Benefiting from the synergistic effects of poly[Se-MI][BF4 ], high efficiencies of 25.10 % and 20.85 % were exhibited by a 0.062-cm2 device and 15.39-cm2 module, respectively. The devices retained over 90 % of their initial efficiency under operation for 2200 h.

4.
Adv Mater ; 35(18): e2300513, 2023 May.
Artículo en Inglés | MEDLINE | ID: mdl-36796414

RESUMEN

Flexible perovskite solar cells (pero-SCs) are the best candidates to complement traditional silicon SCs in portable power applications. However, their mechanical, operational, and ambient stabilities are still unable to meet the practical demands because of the natural brittleness, residual tensile strain, and high defect density along the perovskite grain boundaries. To overcome these issues, a cross-linkable monomer TA-NI with dynamic covalent disulfide bonds, H-bonds, and ammonium is carefully developed. The cross-linking acts as "ligaments" attached on the perovskite grain boundaries. These "ligaments" consisting of elastomers and 1D perovskites can not only passivate the grain boundaries and enhance moisture resistance but also release the residual tensile strain and mechanical stress in 3D perovskite films. More importantly, the elastomer can repair bending-induced mechanical cracks in the perovskite film because of dynamic self-healing characteristics. The resultant flexible pero-SCs exhibit promising improvements in efficiency, and record values (23.84% and 21.66%) are obtained for 0.062 and 1.004 cm2  devices; the flexible devices also show overall improved stabilities with T90  >20 000 bending cycles, operational stability with T90  >1248 h, and ambient stability (relative humidity = 30%) with T90  >3000 h. This strategy paves a new way for the industrial-scale development of high-performance flexible pero-SCs.

5.
Adv Mater ; 35(6): e2208604, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36440601

RESUMEN

The charge carriers of single-junction solar cells can be fluently extracted and then collected by electrodes, leading to weak charge carrier accumulation and low energy loss (Eloss ). However, in tandem solar cells (TSCs), it is a considerable challenge to obtain a balance between the densities of the holes and electrons extracted from the two respective subcells to facilitate an efficient recombination in the interconnecting layer (ICL). Herein, a charge-carrier-dynamic management strategy for inorganic perovskite/organic TSCs is proposed, centered on the simultaneous regulation of the defect states of CsPbI1.9 Br1.1 perovskite in the front subcell and hole transport ability from the perovskite to ICL. The target hole density on the perovskite surface and the hole loss before reaching the ICL are significantly improved. As a result, the hole/electron density offset in the ICL can be effectively narrowed, leading to a balanced charge carrier recombination, which reduces the Eloss in TSCs. The resulting inorganic perovskite/organic 0.062-cm2 TSC exhibits a remarkable power conversion efficiency (PCE) of 23.17% with an ultrahigh open-circuit voltage (Voc ) of 2.15 V, and the PCE of the 1.004-cm2 device (21.69%) exhibited a weak size-dependence. This charge-carrier-dynamic management strategy can also effectively enhance the operational and ultraviolet-light stabilities of the TSCs.

6.
Sci Bull (Beijing) ; 67(12): 1243-1252, 2022 Jun 30.
Artículo en Inglés | MEDLINE | ID: mdl-36546154

RESUMEN

Perovskite solar cells (pero-SCs) performance is essentially limited by severe non-radiative losses and ion migration. Although numerous strategies have been proposed, challenges remain in the basic understanding of their origins. Here, we report a dielectric-screening-enhancement effect for perovskite defects by using organic semiconductors with finely tuned molecular structures from the atoms level. Our method produced various perovskite films with high dielectric constant values, reduced charge capture regions, suppressed ion migration, and it provides an efficient charge transport pathway for suppressing non-radiative recombination beyond the passivation effect. The resulting pero-SCs showed a promising power conversion efficiency (PCE) of 23.35% with a high open-circuit voltage (1.22 V); and the 1-cm2 pero-SCs maintained an excellent PCE (21.93%), showing feasibility for scalable fabrication. The robust operational and thermal stabilities revealed that this method paved a new way to understand the degradation mechanism of pero-SCs, promoting the efficiency, stability and scaled fabrication of the pero-SCs.

7.
Angew Chem Int Ed Engl ; 61(42): e202210613, 2022 Oct 17.
Artículo en Inglés | MEDLINE | ID: mdl-36064999

RESUMEN

Dopant-free organic hole transport materials (HTMs) remain highly desirable for stable and efficient n-i-p perovskite solar cells (pero-SCs) but rarely succeed. Here, we propose a molecular assembly strategy to overcome the limited optoelectronic properties of organic HTMs by precisely designing a linear organic small molecule BDT-DPA-F from the atomic to the molecular levels. BDT-DPA-F can assemble into a fibril network, showing an obviously improved hole mobility and decreased energy disorder. The resultant pero-SCs showed a promising efficiency of 23.12 % (certified 22.48 %), which is the highest certified value of pero-SCs with dopant-free HTMs, to date. These devices also showed a weak-dependence of efficiency on size, enabling a state-of-the-art efficiency of 22.50 % for 1-cm2 device and 20.17 % for 15.64-cm2 module. For the first time, the pero-SCs based on dopant-free HTMs realized ultralong stabilities with T80 lifetimes over 1200 h under operation or thermal aging at 85 °C.

8.
Adv Mater ; 34(14): e2110482, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35122342

RESUMEN

The built-in electric field (BEF) intensity of silicon heterojunction solar cells can be easily enhanced by selective doping to obtain high power conversion efficiencies (PCEs), while it is challenging for perovskite solar cells (pero-SCs) because of the difficulty in doping perovskites in a controllable way. Herein, an effective method is reported to enhance the BEF of FA0.92 MA0.08 PbI3 perovskite by doping an organic ferroelectric material, poly(vinylidene fluoride):dabcoHReO4 (PVDF:DH) with high polarizability, that can be driven even by the BEF of the device itself. The polarization of PVDF:DH produces an additional electric field, which is maintained permanently, in a direction consistent with that of the BEF of the pero-SC. The BEF superposition can more sufficiently drive the charge-carrier transport and extraction, thus suppressing the nonradiative recombination occurring in the pero-SCs. Moreover, the PVDF:DH dopant benefits the formation of a mesoporous PbI2 film, via a typical two-step processing method, thereby promoting perovskite growth with high crystallinity and a few defects. The resulting pero-SC shows a promising PCE of 24.23% for a 0.062 cm2 device (certified PCE of 23.45%), and a remarkable PCE of 22.69% for a 1 cm2 device, along with significantly improved moisture resistances and operational stabilities.

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