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1.
Small ; : e2401487, 2024 May 20.
Article in English | MEDLINE | ID: mdl-38767498

ABSTRACT

Reducing the defect density of perovskite films during the crystallization process is critical in preparing high-performance perovskite solar cells (PSCs). Here, a multi-functional molecule, 3-phenyl-4-aminobutyric acid hydrochloride (APH), with three functional groups including a benzene ring, ─NH3 + and ─COOH, is added into the perovskite precursor solution to improve perovskite crystallization and device performance. The benzene ring increases the hydrophobicity of perovskites, while ─NH3 + and ─COOH passivate defects related to I- and Pb2+, respectively. Consequently, the power conversion efficiency (PCE) of the optimal device increased to 24.65%. Additionally, an effective area of 1 cm2 with a PCE of 22.45% is also prepared using APH as an additive. Furthermore, PSCs prepared with APH exhibit excellent stability by 87% initial PCE without encapsulation after exposure at room temperature under 25% humidity for 5000 h and retaining 70% of initial PCE after aging at 85 °C in an N2 environment for 864 h.

2.
Angew Chem Int Ed Engl ; : e202404401, 2024 May 10.
Article in English | MEDLINE | ID: mdl-38729917

ABSTRACT

It is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high-quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found DFA reacts with DMSO by forming two molecules, difluoroacetate thioether ester (DTE) and difluoroacetic acid (DA). The strong bonding DTE⋅PbI2 and DA⋅PbI2 retard perovskite crystallization process for high-quality film formation, which was monitored through in situ UV/Vis and PL tests. By using DFA additives, we prepared perovskite films with high-quality and low defects. Finally, a champion PCE of 25.28 % was achieved with excellent environmental stability, which retained 95.75 % of the initial PCE after 1152 h at 25 °C under 25 % RH.

3.
Small ; 19(45): e2303017, 2023 Nov.
Article in English | MEDLINE | ID: mdl-37480182

ABSTRACT

With better light utilization, larger tolerance factor, and higher power conversion efficiency (PCE), the HC(NH2 )2 + (FA)-based perovskite is proven superior to the popular CH3 NH3 + (MA)- and Cs-based halide perovskites in solar cell applications. Unfortunately, limited by intrinsic defects within the FA-based perovskite films, the perovskite films can be easily transformed into a yellow δ-phase at room temperature in the fabrication process, a troublesome challenge for its further development. Here, ytterbium fluoride (YbF3 ) is introduced into the perovskite precursor for three objectives. First of all, the partial substitution of Yb3+ for Pb2+ in the perovskite lattice increases the tolerance factor of the perovskite lattice and facilitates the formation of the α phase. Second, YbF3 and DMSO in the solvent form a Lewis acid complex YbF3 ·DMSO, which can passivate the perovskite film, reduce defects, and improve device stability. Consequently, the YbF3 modified Perovskite solar cell exhibits a champion conversion efficiency of 24.53% and still maintains 90% of its initial efficiency after 60 days of air exposure under 30% relative humidity.

4.
Angew Chem Int Ed Engl ; 62(11): e202216668, 2023 Mar 06.
Article in English | MEDLINE | ID: mdl-36593561

ABSTRACT

Wide-band gap (1.68 eV) perovskite solar cells (PSCs) are important components of perovskite/Si tandem devices. However, the efficiency of wide band gap PSCs has been limited by their huge open-circuit voltage (Voc ) deficit due to non-radiative recombination. Deep-level acceptor defects are identified as the major killers of Voc , and they can be effectively improved by passivation with ammonium salts. Theoretical calculation predicts that increasing the distance between F and -NH3 + of fluorinated ammonium can dramatically enhance the electropositivity of -NH3 + terminals, thus providing strong adsorption onto the negatively charged IA and IPb anti-site defects. Characterizations further confirm that surface gradient passivation employing p-FPEAI demonstrates the most efficient passivation effect. Consequently, a record-efficiency of 21.63 % with the smallest Voc deficit of 441 mV is achieved for 1.68 eV-band gap inverted PSCs. Additionally, a flexible PSC and 1 cm2 opaque device also deliver the highest PCEs of 21.02 % and 19.31 %, respectively.

5.
Angew Chem Int Ed Engl ; 62(41): e202309398, 2023 Oct 09.
Article in English | MEDLINE | ID: mdl-37624069

ABSTRACT

Photovoltaic technology with low weight, high specific power in cold environments, and compatibility with flexible fabrication is highly desired for near-space vehicles and polar region applications. Herein, we demonstrate efficient low-temperature flexible perovskite solar cells by improving the interfacial contact between electron-transport layer (ETL) and perovskite layer. We find that the adsorbed oxygen active sites and oxygen vacancies of flexible tin oxide (SnO2 ) ETL layer can be effectively decreased by incorporating a trace amount of titanium tetrachloride (TiCl4 ). The effective defects elimination at the interfacial increases the electron mobility of flexible SnO2 layer, regulates band alignment at the perovskite/SnO2 interface, induces larger perovskite crystal growth, and improves charge collection efficiency in a complete solar cell. Correspondingly, the improved interfacial contact transforms into high-performance solar cells under one-sun illumination (AM 1.5G) with efficiencies up to 23.7 % at 218 K, which might open up a new era of application of this emerging flexible photovoltaic technology to low-temperature environments such as near-space and polar regions.

6.
J Gene Med ; 24(1): e3334, 2022 01.
Article in English | MEDLINE | ID: mdl-33789359

ABSTRACT

BACKGROUND: Glioma stem-like cells (GSCs) are greatly responsible for the progression of glioma. Long noncoding RNAs (lncRNAs) play an important role in glioma tumor progression. This study aims to explore the role and underlying mechanism of lncRNA SNHG9 in regulating GSC cell growth. METHODS: GSCs were obtained from glioma cells (U87 and U251) and referred to as GSC-87 and GSC-251, respectively. The interactions between miR-326 and SNHG9 or SOX9 were analyzed using luciferase reporter assay. Cell growth of GSCs was evaluated by EdU assay and sphere formation assay. RESULTS: SNHG9 expression was significantly higher in GSC-87 and GSC-251 cells than in U87 and U251 cells. SNHG9 overexpression promoted GSC cell growth, whereas SNHG9 knockdown inhibited GSC cell growth. Mechanistically, SNHG9 acted as a competitive endogenous RNA of miR-326 to elevate the expression of SOX9, a direct target of miR-326. Moreover, transfection with miR-326 inhibitor counteracted SNHG9 knockdown-mediated inhibition of GSC cell growth. CONCLUSIONS: SNHG9 facilitates growth of GSCs via the miR-326/SOX9 axis. This study provides a promising therapeutic target for glioma treatment.


Subject(s)
Brain Neoplasms , Glioma , MicroRNAs , Neoplastic Stem Cells , RNA, Long Noncoding , SOX9 Transcription Factor , Brain Neoplasms/genetics , Brain Neoplasms/pathology , Cell Line, Tumor , Cell Proliferation/genetics , Gene Expression Regulation, Neoplastic , Glioma/pathology , Humans , MicroRNAs/genetics , MicroRNAs/metabolism , Neoplastic Stem Cells/metabolism , Neoplastic Stem Cells/pathology , RNA, Long Noncoding/genetics , RNA, Long Noncoding/metabolism , SOX9 Transcription Factor/genetics , SOX9 Transcription Factor/metabolism
7.
Small ; 17(36): e2100955, 2021 09.
Article in English | MEDLINE | ID: mdl-34319656

ABSTRACT

Herein, alkoxylation chemistry is introduced as a "one-stone-three-birds" solution for exploring a new family of highly-fluorescent octupolar 2D-conjugated organic polymers/frameworks (OCOPs/OCOFs) combining far-red emission, high fluorescence quantum yield (QY), and strong two-photon absorption (TPA). Both alkoxy-substituted OCOP and OCOF comprising acrylonitrile-bridged strongly-coupled donor3-(acceptor core) chromophores densely packed in either disordered or ordered forms, exhibit significantly redshifted emission. They produce high QY of 22.2% and 27.8% in tetrahydrofuran, large TPA cross section of 600 and 1124 GM, and 2-3 folds and 15-30 folds that of non-alkoxylate amorphous counterpart respectively. Combined theoretical and experimental studies reveal unique "one-stone-three-birds" role of the alkoxylation in realizing red-shifted-emission, improved QY and TPA enabled by inducing steric hindrance effect for weakened π-π stacking, and triggering p-π conjugation effect for electronically engineering octupolar chromophores, while the crystalline engineering enables enforced coplanarity conformation and improved π-electron delocalization for further improved QY and TPA. The robust and biocompatible pentoxy-substituted polymer can be used not only as metal-free red-emissive phosphor for efficient warm white light-emitting diodes, but also as efficient two-photon fluorescence probes for bio-imaging.


Subject(s)
Acrylonitrile , Polymers , Electrons , Photons , Spectrometry, Fluorescence
8.
Angew Chem Int Ed Engl ; 60(8): 4238-4244, 2021 Feb 19.
Article in English | MEDLINE | ID: mdl-33156572

ABSTRACT

Surface defects have been a key constraint for perovskite photovoltaics. Herein, 1,3-dimethyl-3-imidazolium hexafluorophosphate (DMIMPF6 ) ionic liquid (IL) is adopted to passivate the surface of a formamidinium-cesium lead iodide perovskite (Cs0.08 FA0.92 PbI3 ) and also reduce the energy barrier between the perovskite and hole transport layer. Theoretical simulations and experimental results demonstrate that Pb-cluster and Pb-I antisite defects can be effectively passivated by [DMIM]+ bonding with the Pb2+ ion on the perovskite surface, leading to significantly suppressed non-radiative recombination. As a result, the solar cell efficiency was increased to 23.25 % from 21.09 %. Meanwhile, the DMIMPF6 -treated perovskite device demonstrated long-term stability because the hydrophobic DMIMPF6 layer blocked moisture permeation.

9.
Adv Mater ; : e2403682, 2024 May 03.
Article in English | MEDLINE | ID: mdl-38701489

ABSTRACT

Functional agents are verified to efficiently enhance device performance of perovskite solar cells (PSCs) through surface engineering. However, the influence of intrinsic characteristics of molecules on final device performance is overlooked. Here, a surface reconstruction strategy is developed to enhance the efficiency of inverted PSCs by mitigating the adverse effects of lead chelation (LC) molecules. Bathocuproine (BCP) is chosen as the representative of LC molecules for its easy accessibility and outstanding optoelectronic properties. During this strategy, BCP molecules on perovskite surface are first dissolved in solvents and then captured specially by undercoordinated Pb2+ ions, preventing adverse n-type doping by the molecules themselves. In this case, the BCP molecule exhibits outstanding passivation effect on perovskite surface, which leads to an obviously increased open-circuit voltage (VOC). Therefore, a record power conversion efficiency of 25.64% for NiOx-based inverted PSCs is achieved, maintaining over 80% of initial efficiency after exposure to ambient condition for ≈1500 h.

10.
Adv Mater ; 36(1): e2306870, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37770027

ABSTRACT

With 40% efficiency under room light intensity, perovskite solar cells (PSCs) will be promising power supplies for low-light applications, particularly for Internet of Things (IoT) devices and indoor electronics, shall they become commercialized. Herein, ß-alaninamide hydrochloride (AHC) is utilized to spontaneously form a layer of 2D perovskite nucleation seeds for improved film uniformity, crystallization quality, and solar cell performance. It is found that the AHC addition indeed improves film quality as demonstrated by better uniformity, lower trap density, smaller lattice stress, and, as a result, a 10-fold increase in charge carrier lifetime. Consequently, not only does the small-area (0.09 cm2 ) PSCs achieve a power conversion efficiency of 42.12%, the large-area cells (1.00 cm2 , and 2.56 cm2 ) attain efficiency as high as 40.93%, and 40.07% respectively. All of these are the highest efficiency values for indoor photovoltaic cells with similar sizes, and more importantly, they represent the smallest efficiency loss due to area scale-up. This work provides a new method to fabricate high-performance indoor PSCs (i-PSCs) for IoT devices with great potential in large-area printing technology.

11.
ACS Appl Mater Interfaces ; 16(3): 3279-3288, 2024 Jan 24.
Article in English | MEDLINE | ID: mdl-38199963

ABSTRACT

Herein, we develop a new intelligent moisture-sensitive hybrid aerogel by evenly embedding a proton-conductive covalent organic framework (COF-2SO3H) into a carboxylated cellulose nanofiber network (CNF-C) for water harvesting and spontaneous sustained electricity production from ambient humidity and human respiration. Our strategy first exploits the "suspending agent" role of CNF-C to stably disperse COF materials in water for forming uniform hierarchical hybrid structures. By utilizing the synergy of COF-2SO3H and CNF-C together with their inherent structure merits and surface group effects, the hybrid aerogel displays increased water uptake and ion conductivity. Upon asymmetric moisturization, it can create a self-maintained moisture gradient to engender a concentration difference for mobile Na+ and H+, resulting in efficient charge separation and diffusion. Thus, the hybrid aerogel-based coin-type generator achieves a continuous output voltage of ∼0.55 V for at least 5 h in ambient environments in contrast to that using pure CNF-C and carbon-based generators with transient voltage response. Intriguingly, the wearable generator with an aerogel in a mask is more sensitive to human respiration and achieves repeatable and reliable self-charge for persistent electricity along with an increased output voltage of up to 1.0 V and much faster self-charge (only 3 min), both of which surpass most reported moisture-enabled generators.


Subject(s)
Electricity , Protons , Humans , Electric Conductivity , Cellulose , Respiration
12.
Adv Mater ; 36(18): e2312041, 2024 May.
Article in English | MEDLINE | ID: mdl-38219020

ABSTRACT

The remarkable progress in perovskite solar cell (PSC) technology has witnessed a remarkable leap in efficiency within the past decade. As this technology continues to mature, flexible PSCs (F-PSCs) are emerging as pivotal components for a wide array of applications, spanning from powering portable electronics and wearable devices to integrating seamlessly into electronic textiles and large-scale industrial roofing. F-PSCs characterized by their lightweight, mechanical flexibility, and adaptability for cost-effective roll-to-roll manufacturing, hold immense commercial potential. However, the persistent concerns regarding the overall stability and mechanical robustness of these devices loom large. This comprehensive review delves into recent strides made in enhancing the mechanical stability of F-PSCs. It covers a spectrum of crucial aspects, encompassing perovskite material optimization, precise crystal grain regulation, film quality enhancement, strategic interface engineering, innovational developed flexible transparent electrodes, judicious substrate selection, and the integration of various functional layers. By collating and analyzing these dedicated research endeavors, this review illuminates the current landscape of progress in addressing the challenges surrounding mechanical stability. Furthermore, it provides valuable insights into the persistent obstacles and bottlenecks that demand attention and innovative solutions in the field of F-PSCs.

13.
Adv Mater ; 36(3): e2305513, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37878999

ABSTRACT

Metal halide perovskite single crystals (MHP-SCs) are known for their facile fabrication into large sizes using inexpensive solution methods. Owing to their combination of large mobility-lifetime products and strong X-ray absorption, they are considered promising materials for efficient X-ray detection. However, they suffer from large dark currents and severe ion migration, which limit their sensitivity and stability in critical X-ray detection applications. Herein, a heterointerface design is proposed to reduce both the dark current and ion migration by forming a heterojunction. In addition, the carrier transport performance is significantly improved using heterointerface engineering by designing a gradient band structure in the SCs. The SC heterojunction detectors exhibit a high sensitivity of 3.98 × 105 µC Gyair -1 cm-2 with a low detection limit of 12.2 nGyair s-1 and a high spatial resolution of 10.2 lp mm-1 during imaging. These values are among the highest reported for state-of-the-art MHP X-ray detectors. Moreover, the detectors show excellent stability under continuous X-ray irradiation and maintainclear X-ray imaging after 240 d. This study provides novel insights into the design and fabrication of X-ray detectors with high detection efficiency and stability, which are beneficial for developing inexpensive, high-resolution X-ray imaging equipment.

14.
Adv Mater ; 36(24): e2311562, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38507724

ABSTRACT

A robust perovskite-buried interface is pivotal for achieving high-performance flexible indoor photovoltaics as it significantly influences charge transport and extraction efficiency. Herein, a molecular bridge strategy is introduced utilizing sodium 2-cyanoacetate (SZC) additive at the perovskite-buried interface to simultaneously achieve in situ passivation of interfacial defects and bottom-up crystallization modulation, resulting in high-performance flexible indoor photovoltaic applications. Supported by both theoretical calculations and experimental evidences, it illustrates how SZCs serve as molecular bridges, establishing robust bonds between SnO2 transport layer and perovskite, mitigating oxygen vacancy defects and under-coordinated Pb defects at interface during flexible fabrication. This, in turn, enhances interfacial energy level alignment and facilitates efficient carrier transport. Moreover, this in situ investigation of perovskite crystallization dynamics reveals bottom-up crystallization modulation, extending perovskite growth at the buried interface and influencing subsequent surface recrystallization. This results in larger crystalline grains and improved lattice strain of the perovskite during flexible fabrication. Finally, the optimized flexible solar cells achieve an impressive efficiency exceeding 41% at 1000 lux, with a fill factor as high as 84.32%. The concept of the molecular bridge represents a significant advancement in enhancing the performance of perovskite-based flexible indoor photovoltaics for the upcoming era of Internet of Things (IoT).

15.
Adv Mater ; 35(18): e2211977, 2023 May.
Article in English | MEDLINE | ID: mdl-36802105

ABSTRACT

Lead-free A3 Bi2 I9 -type perovskites are demonstrated as a class of promising semiconductors for high-performance X-ray detection due to their high bulk resistivity and strong X-ray absorption, as well as reduced ion migration. However, due to their long interlamellar distance along their c-axis, their limited carrier transport along the vertical direction is a bottleneck for their detection sensitivity. Herein, a new A-site cation of aminoguanidinium (AG) with all-NH2 terminals is designed to shorten the interlayer spacing by forming more and stronger NH···I hydrogen bonds. The prepared large AG3 Bi2 I9 single crystals (SCs) render shorter interlamellar distance for a larger mobility-lifetime product of 7.94 × 10-3  cm2  V-1 , which is three times higher than the value measured on the best MA3 Bi2 I9 SC (2.87 × 10-3  cm2  V-1 ). Therefore, the X-ray detectors fabricated on the AG3 Bi2 I9 SC exhibit high sensitivity of 5791 uC Gy-1  cm-2 , a low detection limit of 2.6 nGy s-1, and a short response time of 690 µs, all of which are far better than those of the state-of-the-art MA3 Bi2 I9 SC detectors. The combination of high sensitivity and high stability enables astonishingly high spatial resolution (8.7 lp mm-1 ) X-ray imaging. This work will facilitate the development of low-cost and high-performance lead-free X-ray detectors.

16.
Sci Adv ; 9(35): eadh2255, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37647409

ABSTRACT

Preliminary theoretical analyses indicate that lattice relaxation may be used to release lattice strain in the FAPbI3 perovskite to warrant both high x-ray detection performance and improved stability. Herein, we demonstrate stable black α-phase FAPbI3 single crystals (SCs) realized by lattice engineering via annealing in the ambient atmosphere. The engineered α-FAPbI3 SC detector shows almost all the best figures of merit including a high sensitivity of 4.15 × 105 µC Gyair-1 cm-2, a low detection limit of 1.1 nGyair s-1, a high resolution of 15.9 lp mm-1, and a short response time of 214 µs. We further demonstrate high-definition x-ray imaging at a dose rate below 10 nGyair s-1 on the FAPbI3 SC, indicating a minimal dose-area product of 0.048 mGyair cm2 to the patient for one-time posteroanterior chest diagnosis, which is more than 3000 times lower than the international reference level of 150 mGyair cm2. In addition, the robust long-term stability enables the FAPbI3 SC x-ray detector to work steadily for more than 40 years.

17.
Materials (Basel) ; 15(7)2022 Mar 31.
Article in English | MEDLINE | ID: mdl-35407885

ABSTRACT

Since 2009, there has been renewed interest in perovskite materials due to the rise of metal halide perovskite photoelectric materials, especially in the field of perovskite solar cells (PSCs) [...].

18.
Adv Sci (Weinh) ; : e2205536, 2022 Dec 01.
Article in English | MEDLINE | ID: mdl-36453564

ABSTRACT

In the past decade, metal halide perovskite (HP) has become a superstar semiconductor material due to its great application potential in the photovoltaic and photoelectric fields. In fact, HP initially attracted worldwide attention because of its excellent photovoltaic efficiency. However, HP and its derivatives also show great promise in X-ray detection due to their strong X-ray absorption, high bulk resistivity, suitable optical bandgap, and compatibility with integrated circuits. In this review, the basic working principles and modes of both the direct-type and the indirect-type X-ray detectors are first summarized before discussing the applicability of HP for these two types of detection based on the pros and cons of different perovskites. Furthermore, the authors expand their view to different preparation methods developed for HP including single crystals and polycrystalline materials. Upon systematically analyzing their potential for X-ray detection and photoelectronic characteristics on the basis of different structures and dimensions (0D, 2D, and 3D), recent progress of HPs (mainly polycrystalline) applied to flexible X-ray detection are reviewed, and their practicability and feasibility are discussed. Finally, by reviewing the current research on HP-based X-ray detection, the challenges in this field are identified, and the main directions and prospects of future research are suggested.

19.
ACS Appl Mater Interfaces ; 14(25): 28729-28737, 2022 Jun 29.
Article in English | MEDLINE | ID: mdl-35699996

ABSTRACT

Organic-inorganic Pb-based halide perovskite photoelectrical materials, especially perovskite solar cells (PSCs), have attracted attention due to the significant efforts in improving the power conversion efficiency (PCE) to above 25%. However, the stability issue of the PSCs restricts their further development for commercialization. Strategies are designed to keep moisture and oxygen out of the perovskite films, such as additive, surface passivation, and solvent engineering; however, usually, the corrosion of active films by the residual solvent is mostly ignored. Solvent residue is the paramount factor influencing the stability of the perovskite film prepared by the solution method, and most solvents can be easily absorbed and accelerate the perovskite film decomposition. Here, we studied the residual solvent effect on two kinds of perovskite films obtained by different annealing processes: hot air annealing and hot bench annealing. Several detection techniques were used to study the performance of two different annealing methods, including time-of-flight secondary ion mass spectrometry (ToF-SIMS), thermogravimetric analysis (TGA), and field-emission scanning electron microscopy (FESEM). The perovskite film obtained by hot air annealing shows less residual solvent and better device performance than the hot bench annealing method. This method is expected to provide insight into reducing solvent residue to improve the stability of the PSCs, especially for future commercialization.

20.
Adv Mater ; 34(24): e2201681, 2022 Jun.
Article in English | MEDLINE | ID: mdl-35435279

ABSTRACT

Flexible perovskite solar cells (f-PSCs) have attracted great attention because of their unique advantages in lightweight and portable electronics applications. However, their efficiencies are far inferior to those of their rigid counterparts. Herein, a novel histamine diiodate (HADI) is designed based on theoretical study to modify the SnO2 /perovskite interface. Systematic experimental results reveal that the HADI serves effectively as a multifunctional agent mainly in three aspects: 1) surface modification to realign the SnO2 conduction band upward to improve interfacial charge extraction; 2) passivating the buried perovskite surface, and 3) bridging between the SnO2 and perovskite layers for effective charge transfer. Consequently, the rigid MA-free PSCs based on the HADI-SnO2 electron transport layer (ETL) display not only a high champion power conversion efficiency (PCE) of 24.79% and open-circuit voltage (VOC ) of 1.20 V but also outstanding stability as demonstrated by the PSCs preserving 91% of their initial efficiencies after being exposed to ambient atmosphere for 1200 h without any encapsulation. Furthermore, the solution-processed HADI-SnO2 ETL formed at low temperature (100 °C) is utilized in f-PSCs that achieve a PCE as high as 22.44%, the highest reported PCE for f-PSCs to date.

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