Two novel wide-bandgap copolymers, PBDT-TDZ and PBDTS-TDZ, are developed based on 1,3,4-thiadiazole (TDZ) and benzo[1,2-b:4,5-b']dithiophene (BDT) building blocks. These copolymers exhibit wide bandgaps over 2.07 eV and low-lying highest occupied molecular orbital (HOMO) levels below -5.35 eV, which match well with the typical low-bandgap acceptor of ITIC, resulting in a good complementary absorption from 300 to 900 nm and a low HOMO level offset (≤0.13 eV). Compared to PBDT-TDZ, PBDTS-TDZ with alkylthio side chains exhibits the stronger optical absorption, lower-lying HOMO level, and higher crystallinity. By using a single green solvent of o-xylene, PBDTS-TDZ:ITIC devices exhibit a large open-circuit voltage (V ) up to 1.10 eV and an extremely low energy loss (E ) of 0.48 eV. At the same time, the desirable high short-circuit current density (J ) of 17.78 mA cm and fill factor of 65.4% are also obtained, giving rise to a high power conversion efficiency (PCE) of 12.80% without any additive and post-treatment. When adopting a homotandem device architecture, the PCE is further improved to 13.35% (certified as 13.19%) with a much larger V of 2.13 V, which is the best value for any type of homotandem organic solar cells reported so far.
Ni-rich cathode materials have drawn lots of attention owing to its high discharge specific capacity and low cost. Nevertheless, there are still some inherent problems that desiderate to be settled, such as cycling stability and rate properties as well as thermal stability. In this article, the conductive polymers that integrate the excellent electronic conductivity of polyaniline (PANI) and the high ionic conductivity of poly(ethylene glycol) (PEG) are designed for the surface modification of LiNiCoMnO cathode materials. Besides, the PANI-PEG polymers with elasticity and flexibility play a significant role in alleviating the volume contraction or expansion of the host materials during cycling. A diversity of characterization methods including scanning electron microscopy, energy-dispersive X-ray spectrometer, transmission electron microscopy, thermogravimetric analysis, Fourier transform infrared have demonstrated that LiNiCoMnO cathode materials is covered with a homogeneous and thorough PANI-PEG polymers. As a result, the surface-modified LiNiCoMnO delivers high discharge specific capacity, excellent rate properties, and outstanding cycling performance.
A novel wide-bandgap copolymer of PBDT-ODZ based on benzo[1,2-b:4,5-b' ]dithiophene (BDT) and 1,3,4-oxadiazole (ODZ) blocks is developed for efficient nonfullerene polymer solar cells (NF-PSCs). PBDT-ODZ exhibits a wide bandgap of 2.12 eV and a low-lying highest occupied molecular orbital (HOMO) level of -5.68 eV, which could match well with the low-bandgap acceptor of 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone)-5,5,11,11-tetrakis(4-hexylthienyl)-dithieno[2,3-d:2',3'-d']-s-indaceno[1,2-b:5,6-b']-dithiophene (ITIC-Th), inducing a good complementary absorption from 300 to 800 nm and a minimal HOMO level offset (0.1 eV). The PBDT-ODZ:ITIC-Th devices exhibit a large open-circuit voltage (V ) of 1.08 eV and a low energy loss (E ) of 0.50 eV, delivering a high power conversion efficiency (PCE) of 10.12%. By adding a small amount of copper(I) iodide (CuI) as an additive to form coordination complexes in the active blends, much higher device performances are achieved due to the improved absorption and crystallinity. After incorporating 4% of CuI, the PCE is elevated to 12.34%, with a V of 1.06 V, a J of 17.1 mA cm and a fill factor of 68.1%. This work not only provides a novel oxadiazole-containing wide-bandgap polymeric donor candidate for high-performance NF-PSCs but also presents an efficient morphology-optimization approach to elevate the PCE of NF-PSCs for future practical applications.
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