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1.
Nanoscale ; 13(47): 20067-20077, 2021 Dec 13.
Article in English | MEDLINE | ID: mdl-34846058

ABSTRACT

Metal halide perovskite quantum dots (QDs) hold great promise as building blocks for next-generation light emitting devices (LEDs). The preparation of perovskite QD films with high photoluminescence quantum yield (PLQY) is the key to realizing efficient LEDs. However, the conventional deposition method of spin-coating of pre-synthesized QD ink solutions results in perovskite QD films with low PLQY (typically <45%) due to non-radiative recombination centers induced in the deposition process. Here, by utilizing the ionic nature and steric hindrance effect of the ionic liquid, we demonstrate an in situ deposition method for perovskite QD films with high PLQY by directly spin-coating precursor solutions containing an ionic liquid. Furthermore, mechanistic study reveals that the ionic liquid not only induces the formation of QDs but also suppresses defect-related recombination through the interaction with uncoordinated metal atoms on the surface of the QDs. As a result, the in situ deposited CsPbBr3 QD film with a PLQY as high as 85.2% and long-term air stability is achieved. These findings demonstrate that the introduction of an ionic liquid provides an effective strategy to enhance the performance of in situ formed perovskite QD films, which could benefit the development of efficient LEDs and other optoelectronic devices.

2.
Nat Commun ; 12(1): 5980, 2021 Oct 13.
Article in English | MEDLINE | ID: mdl-34645825

ABSTRACT

While self-healing is considered a promising strategy to achieve long-term stability for oxygen evolution reaction (OER) catalysts, this strategy remains a challenge for OER catalysts working in highly alkaline conditions. The self-healing of the OER-active nickel iron layered double hydroxides (NiFe-LDH) has not been successful due to irreversible leaching of Fe catalytic centers. Here, we investigate the introduction of cobalt (Co) into the NiFe-LDH as a promoter for in situ Fe redeposition. An active borate-intercalated NiCoFe-LDH catalyst is synthesized using electrodeposition and shows no degradation after OER tests at 10 mA cm-2 at pH 14 for 1000 h, demonstrating its self-healing ability under harsh OER conditions. Importantly, the presence of both ferrous ions and borate ions in the electrolyte is found to be crucial to the catalyst's self-healing. Furthermore, the implementation of this catalyst in photoelectrochemical devices is demonstrated with an integrated silicon photoanode. The self-healing mechanism leads to a self-limiting catalyst thickness, which is ideal for integration with photoelectrodes since redeposition is not accompanied by increased parasitic light absorption.

3.
J Phys Chem Lett ; 12(10): 2668-2675, 2021 Mar 18.
Article in English | MEDLINE | ID: mdl-33689369

ABSTRACT

Due to the ultrafast crystallization process in the triple-source ligand-assisted reprecipitation (TSLARP) technique the [LyPbBrx] octahedra is easily distorted, resulting in anisotropic two-dimensional nanoplatelets (NPLs) with low photoluminescence quantum yield (PLQY) and poor stability. Unexpectedly, we obtain CsPbBr3 NPLs with PLQY approaching unity and high stability using the TSLARP technique through aging the metal-oleate precursors. We find that the significant enhancement of the PLQY is related to the change of solution chemistry of the Pb-oleate precursor in the aging process. While hybrid CsPbBr3@Cs4PbBr6 NPLs with low PLQY (28%) are formed with fresh Pb-oleate precursor, phase-pure CsPbBr3 NPLs with PLQY of 97.4% are obtained with the aged Pb-oleate precursor. A model that takes into account the transformation of the Pb-oleate in toluene from isolated molecules into clusters after aging is proposed to explain the phenomenon. Our finding highlights the importance of understanding the solution chemistry for the synthesis of the highly luminescent NPLs and provides a new way to break the "blue-wall" in perovskite light-emitting devices.

4.
J Phys Chem Lett ; 10(20): 6382-6388, 2019 Oct 17.
Article in English | MEDLINE | ID: mdl-31593470

ABSTRACT

Organic-free perovskite solar cells (PSCs) have been considered as the most promising candidate for achieving long-term stability. Here, we demonstrate an organic-free PSC consisting of inorganic CsPbI2Br perovskite, nickel oxide hole transport layer, and niobium oxide electron transport layer. A maximum power conversion efficiency (PCE) of 11.20% is achieved with an active area of 5 cm2, and it increases to 14.11% with smaller area. More importantly, the organic-free PSCs show excellent thermal stability with PCE remaining above 98% of its initial value when heated at 100 °C for 150 min. Postannealing at a proper temperature further increases its maximum PCE to 14.45%, which is the highest among any reported all-inorganic PSCs with a p-i-n structure. The enhanced performance of the postannealed device is ascribed to the decreased trap-state density and improved interface charge-transfer properties. These results demonstrated that this novel organic-free device architecture can be employed to fabricate efficient and stable PSCs for large-scale manufacturing.

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