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1.
ACS Appl Mater Interfaces ; 14(33): 37990-38003, 2022 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-35904802

RESUMO

In this study, we synthesized four new A-DA'D-A acceptors (where A and D represent acceptor and donor chemical units) incorporating perylene diimide units (A') as their core structures and presenting various modes of halogenation and substitution of the functional groups at their end groups (A). In these acceptors, by fusing dithiophenepyrrole (DTP) moieties (D) to the helical perylene diimide dimer (hPDI) to form fused-hPDI (FhPDI) cores, we could increase the D/A' oscillator strength in the cores and, thus, the intensity of intramolecular charge transfer (ICT), thereby enhancing the intensity of the absorption bands. With four different end group units─IC2F, IC2Cl, IO2F, and IO2Cl─tested, each of these acceptor molecules exhibited different optical characteristics. Among all of these systems, the organic photovoltaic device incorporating the polymer PCE10 blended with the acceptor FhPDI-IC2F (1:1.1 wt %) had the highest power conversion efficiency (PCE) of 9.0%; the optimal PCEs of PCE10:FhPDI-IO2F, PCE10:FhPDI-IO2Cl, and PCE10:FhPDI-IC2Cl (1:1.1 wt %) devices were 5.2, 4.7, and 7.7%, respectively. The relatively high PCE of the PCE10:FhPDI-IC2F device resulted primarily from the higher absorption coefficients of the FhPDI-IC2F acceptor, lower energy loss, and more efficient charge transfer; the FhPDI-IC2F system experienced a lower degree of geminate recombination─as a result of improved delocalization of π-electrons along the acceptor unit─relative to that of the other three acceptors systems. Thus, altering the end groups of multichromophoric PDI units can increase the PCEs of devices incorporating PDI-derived materials and might also be a new pathway for the creation of other valuable fused-ring derivatives.

2.
Small ; 18(19): e2107881, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35417059

RESUMO

In contrast to the 2D organic-inorganic hybrid Ruddlesden-Popper halide perovskites (RPP), a new class of 2D all inorganic RPP (IRPP) has been recently proposed by substituting the organic spacers with an optimal inorganic alternative of cesium cations (Cs+ ). Nevertheless, the synthesis of high-membered 2D IRPPs (n > 1) has been a very challenging task because the Cs+ need to act as both spacers and A-site cations simultaneously. This work presents the successful synthesis of stable phase-pure high-membered 2D IRPPs of Csn+1 Pbn Br3n+1 nanosheets (NSs) with n = 3 and 4 by employing the strategy of using additional strong binding bidentate ligands. The structures of the 2D IRPPs (n = 3 and 4) NSs are confirmed by powder X-ray diffraction and high-resolution aberration-corrected scanning transmission electron microscope measurements. These 2D IRPPs NSs exhibit a strong quantum confinement effect with tunable absorption and emission in the visible light range by varying their n values, attributed to their inherent 2D quantum-well structure. The superior structural and optical stability of the phase-pure high-membered 2D IRPPs make them a promising candidate as photocatalysts in CO2 reduction reactions with outstanding photocatalytic performance and long-term stability.

3.
Nano Lett ; 19(8): 5053-5061, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31298866

RESUMO

Solution-processed organic photovoltaics (OPVs) based on bulk-heterojunctions have gained significant attention to alleviate the increasing demend of fossil fuel in the past two decades. OPVs combined of a wide bandgap polymer donor and a narrow bandgap nonfullerene acceptor show potential to achieve high performance. However, there are still two reasons to limit the OPVs performance. One, although this combination can expand from the ultraviolet to the near-infrared region, the overall external quantum efficiency of the device suffers low values. The other one is the low open-circuit voltage (VOC) of devices resulting from the relatively downshifted lowest unoccupied molecular orbital (LUMO) of the narrow bandgap. Herein, the approach to select and incorporate a versatile third component into the active layer is reported. A third component with a bandgap larger than that of the acceptor, and absorption spectra and LUMO levels lying within that of the donor and acceptor, is demonstrated to be effective to conquer these issues. As a result, the power conversion efficiencies (PCEs) are enhanced by the elevated short-circuit current and VOC; the champion PCEs are 11.1% and 13.1% for PTB7-Th:IEICO-4F based and PBDB-T:Y1 based solar cells, respectively.

4.
ACS Appl Mater Interfaces ; 9(16): 14006-14012, 2017 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-28281352

RESUMO

Ink-printing method emerges as a viable way for manufacturing large-scale flexible Cu(In,Ga)Se2 (CIGS) thin film photovoltaic (TFPV) devices owing to its potential for the rapid process, mass production, and low-cost nonvacuum device fabrication. Here, we brought the femtosecond laser annealing (fs-LA) process into the ink-printing CIGS thin film preparation. The effects of fs-LA treatment on the structural and optoelectronic properties of the ink-printing CIGS thin films were systematically investigated. It was observed that, while the film surface morphology remained essentially unchanged under superheating, the quality of crystallinity was significantly enhanced after the fs-LA treatment. Moreover, a better stoichiometric composition was achieved with an optimized laser scanning rate of the laser beam, presumably due to the much reduced indium segregation phenomena, which is believed to be beneficial in decreasing the defect states of InSe, VSe, and InCu. Consequently, the shunt leakage current and recombination centers were both greatly decreased, resulting in a near 20% enhancement in photovoltaic conversion efficiency.

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