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1.
Angew Chem Int Ed Engl ; 63(27): e202403264, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38659076

RESUMEN

In situ cyclized polyacrylonitrile (CPAN) is developed to replace n-type metal oxide semiconductors (TiO2 or SnO2) as an electron selective layer (ESL) for highly efficient and stable n-i-p perovskite solar cells (PSCs). The CPAN layer is fabricated via facile in situ cyclization reaction of polyacrylonitrile (PAN) coated on a conducting glass substrate. The CPAN layer is robust and insoluble in common solvents, and possesses n-type semiconductor properties with a high electron mobility of 4.13×10-3 cm2 V-1 s-1. With the CPAN as an ESL, the PSC affords a power conversion efficiency (PCE) of 23.12 %, which is the highest for the n-i-p PSCs with organic ESLs. Moreover, the device with the CPAN layer holds superior operational stability, maintaining over 90 % of their initial efficiency after 500 h continuous light soaking. These results confirm that the CPAN layer would be a desirable low-cost and efficient ESL for n-i-p PSCs and other photoelectronic devices with high performance and stability.

2.
J Am Chem Soc ; 145(10): 5872-5879, 2023 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-36872583

RESUMEN

Passivating defects using organic halide salts, especially chlorides, is an effective method to improve power conversion efficiencies (PCEs) of perovskite solar cells (PSCs) arising from the stronger Pb-Cl bonding than Pb-I and Pb-Br bonding. However, Cl- anions with a small radius are prone to incorporation into the perovskite lattice that distorts the lead halide octahedron, degrading the photovoltaic performance. Here, we substitute atomic-Cl-containing organic molecules for widely used ionic-Cl salts, which not only retain the efficient passivation by Cl but also prevent the incorporation of Cl into the bulk lattice, benefiting from the strong covalent bonding between Cl atoms and organic frameworks. We find that only when the distance of Cl atoms in single molecules matches well with the distance of halide ions in perovskites can such a configuration maximize the defect passivation. We thereby optimize the molecular configuration to enable multiple Cl atoms in an optimal spatial position to maximize their binding with surface defects. The resulting PSCs achieve a certified PCE of 25.02%, among the highest PCEs for PSCs, and retain 90% of their initial PCE after 500 h of continuous operation.

3.
Org Biomol Chem ; 12(8): 1232-6, 2014 Feb 28.
Artículo en Inglés | MEDLINE | ID: mdl-24435259

RESUMEN

An improved protocol was described for the amination of chloroarenes with diarylamines under NiCl2(PCy3)2 catalysis in the presence of a Grignard reagent as base. This method fully suits bromo-/iodoarene substrates as well, and even is expanded to certain aryl tosylates. A preliminary investigation into the mechanism suggests that this amination reaction might proceed through Ni(I) and Ni(III) intermediates rather than via the usually expected Ni(0)-Ni(II) cycle.

4.
J Colloid Interface Sci ; 646: 824-833, 2023 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-37230000

RESUMEN

With the complexity and diversification of thermoelectric (TE) application scenarios, it becomes increasingly difficult for single-component thermoelectric materials to satisfy practical demands. Therefore, recent researches have largely focused on the development of the multi-component nanocomposites, which are probably a good solution for the TE application of some materials that are not eligible when used alone. In this work, a seires of single-walled carbon nanotube (SWCNT)/polypyrrole (PPy)/tellurium (Te)/lead telluride (PbTe) multi-layer flexible composite films were fabricated via the successive electrodeposition of the flexible PPy layer with a low thermal conductivity, the ultra-thin Te induction layer, and the brittle PbTe layer with a large Seebeck coefficient over the pre-fabricated SWCNT membrane electrode with a high electrical conductivity. Through the complementary advantages between different components and the multiple synergies of the interface engineering, the SWCNT/PPy/Te/PbTe composites harvested the excellent TE performance with a maximum power factor (PF) of 929.8 ± 35.4 µW m-1 K-2 at room temperature, outperforming those of most of the electrochemically-prepared organic/inorganic TE composites reported previously. This work evidenced that the electrochemical multi-layer assembly is a feasible tactic for constructing special thermoelectric materials to meet customized requirements, which could also be applied to other material platforms.

5.
ACS Appl Mater Interfaces ; 14(8): 10815-10824, 2022 Mar 02.
Artículo en Inglés | MEDLINE | ID: mdl-35175746

RESUMEN

As one of the most attractive inorganics to improve the thermoelectric (TE) performance of the conducting polymers, tellurium (Te) has received intense concern due to its superior Seebeck coefficient (S). However, far less attention has been paid to polypyrrole (PPy)/Te TE composites to date. In this work, we present an innovative full-electrochemical method to architect PPy/Te TE composite films by sequentially depositing Te with large S and PPy with high electrical conductivity (σ). Consequently, the PPy/Te composite films achieved excellent TE performance, with the largest power factor (PF) reaching up to 234.3 ± 4.1 µW m-1 K-2. To the best of our knowledge, this value approaches the reported highest PF record (240.3 ± 5.0 µW m-1 K-2) for PPy-based composites. This suggests that the modified full-electrochemical method is a feasible and effective strategy for achieving high-performance TE composite films, which would probably provide a general guideline for the design and preparation of excellent TE materials in the future.

6.
RSC Adv ; 11(15): 8664-8673, 2021 Feb 23.
Artículo en Inglés | MEDLINE | ID: mdl-35423352

RESUMEN

Organic polymer/inorganic particle composites with thermoelectric (TE) properties have witnessed rapid progress in recent years. Nevertheless, both development of novel polymers and optimization of compositing methods remain highly desirable. In this study, we first demonstrated a simulated in situ coagulation strategy for construction of high-performance thermoelectric materials by utilizing single-walled carbon nanotubes (SWCNTs) and a new D-A polymer TPO-TTP12 that was synthesized via incorporating dioxothiopyrone subunit into a polymeric chain. It was proven that the preparation methods have a significant influence on thermoelectric properties of the TPO-TTP12/SWCNT composites. The in situ prepared composite films tend to achieve much better thermoelectric performances than those prepared by simply mixing the corresponding polymer with SWCNTs. As a result, the in situ compositing obtains the highest Seebeck coefficient of 66.10 ± 0.05 µV K-1 at the TPO-TTP12-to-SWCNT mass ratio of 1/2, and the best electrical conductivity of up to 500.5 ± 53.3 S cm-1 at the polymer/SWCNT mass ratio of 1/20, respectively; moreover, the power factor for the in situ prepared composites reaches a maximum value of 141.94 ± 1.47 µW m-1 K-2, far higher than that of 104.68 ± 0.86 µW m-1 K-2 for the by-mixing produced composites. This indicates that the dioxothiopyrone moiety is a promising building block for constructing thermoelectric polymers, and the simulated in situ compositing strategy is a promising way to improve TE properties of composite materials.

7.
RSC Adv ; 11(35): 21754-21759, 2021 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-35478793

RESUMEN

Solution-processable organic-inorganic hybrid perovskites are being widely investigated for many applications, including solar cells, light-emitting diodes, photodetectors, and lasers. Herein, we report, for the first time, successful fabrication of xerographic photoreceptors using methylammonium lead iodide (CH3NH3PbI3) perovskite as a light-absorbing material. With the incorporation of polyethylene glycol (PEG) into the perovskite film, the ion migration inherent to the perovskite material can be effectively suppressed, and the resulting photoreceptor exhibits a high and panchromatic photosensitivity, large surface potential, low dark decay, and high environmental resistance and electrical cycling stability. Specifically, the energies required to photodischarge one half of the initial surface potential (E 0.5) are 0.074 µJ cm-2 at 550 nm and 0.14 µJ cm-2 at 780 nm, respectively. The photosensitivites outmatch those of the conventionally used organic pigments having narrow spectral responses. Our findings inform a new generation of highly efficient and low-cost xerographic photoreceptors based on perovskite materials.

8.
RSC Adv ; 9(61): 35913-35916, 2019 Oct 31.
Artículo en Inglés | MEDLINE | ID: mdl-35528057

RESUMEN

A simple, mild and efficient protocol was developed for the alkylation of fluorene with alcohols in the presence of t-BuOK as catalyst, affording the desired 9-monoalkylfluorenes with near quantitative yields in most cases.

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