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1.
Angew Chem Int Ed Engl ; 62(30): e202305815, 2023 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-37227157

RESUMEN

Halide-related surface defects on inorganic halide perovskite not only induce charge recombination but also severely limit the long-term stability of perovskite solar cells. Herein, adopting density functional theory calculation, we verify that iodine interstitials (Ii ) has a low formation energy similar to that of the iodine vacancy (VI ) and is also readily formed on the surface of all-inorganic perovskite, and it is regarded to function as an electron trap. We screen a specific 2,6-diaminopyridine (2,6-DAPy) passivator, which, with the aid of the combined effects from halogen-Npyridine and coordination bonds, not only successfully eliminates the Ii and dissociative I2 but also passivates the abundant VI . Furthermore, the two symmetric neighboring -NH2 groups interact with adjacent halides of the octahedral cluster by forming hydrogen bonds, which further promotes the adsorption of 2,6-DAPy molecules onto the perovskite surface. Such synergetic effects can significantly passivate harmful iodine-related defects and undercoordinated Pb2+ , prolong carrier lifetimes and facilitate the interfacial hole transfer. Consequently, these merits enhance the power-conversion efficiency (PCE) from 19.6 % to 21.8 %, the highest value for this type of solar cells, just as importantly, the 2,6-DAPy-treated CsPbI3-x Brx films show better environmental stability.

2.
Angew Chem Int Ed Engl ; 62(6): e202216634, 2023 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-36480237

RESUMEN

Minimizing surface defect is vital to further improve power conversion efficiency (PCE) and stability of inorganic perovskite solar cells (PSCs). Herein, we designed a passivator trifluoroacetamidine (TFA) to suppress CsPbI3-x Brx film defects. The amidine group of TFA can strongly chelate onto the perovskite surface to suppress the iodide vacancy, strengthened by additional hydrogen bonds. Moreover, three fluorine atoms allow strong intermolecular connection via intermolecular hydrogen bonds, thus constructing a robust shield against moisture. The TFA-treated PSCs exhibit remarkably suppressed recombination, yielding the record PCEs of 21.35 % and 17.21 % for 0.09 cm2 and 1.0 cm2 device areas, both of which are the highest for all-inorganic PSCs so far. The device also achieves a PCE of 39.78 % under indoor illumination, the highest for all-inorganic indoor photovoltaic devices. Furthermore, TFA greatly improves device ambient stability by preserving 93 % of the initial PCE after 960 h.

3.
Angew Chem Int Ed Engl ; 62(41): e202309398, 2023 Oct 09.
Artículo en Inglés | MEDLINE | ID: mdl-37624069

RESUMEN

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.

4.
Adv Mater ; 36(9): e2307583, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-37824785

RESUMEN

The critical requirement for ambient-printed formamidinium lead iodide (FAPbI3 ) lies in the control of nucleation-growth kinetics and defect formation behavior, which are extensively influenced by interactions between the solvent and perovskite. Here, a strategy is developed that combines a cosolvent and an additive to efficiently tailor the coordination between the solvent and perovskite. Through in situ characterizations, the direct crystallization from the sol-gel phase to α-FAPbI3 is illustrated. When the solvent exhibits strong interactions with the perovskite, the sol-gel phases cannot effectively transform into α-FAPbI3 , resulting in a lower nucleation rate and confined crystal growth directions. Consequently, it becomes challenging to fabricate high-quality void-free perovskite films. Conversely, weaker solvent-perovskite coordination promotes direct crystallization from sol-gel phases to α-FAPbI3 . This process exhibits more balanced nucleation-growth kinetics and restrains the formation of defects and microstrains in situ. This strategy leads to improved structural and optoelectronic properties within the FAPbI3 films, characterized by more compact grain stacking, smoother surface morphology, released lattice strain, and fewer defects. The ambient-printed FAPbI3 perovskite solar cells fabricated using this strategy exhibit a remarkable power conversion efficiency of 24%, with significantly reduced efficiency deviation and negligible decreases in the stabilized output.

5.
Adv Mater ; 36(24): e2311562, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38507724

RESUMEN

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).

6.
Adv Mater ; 36(23): e2312014, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38380583

RESUMEN

Perovskite photovoltaics have emerged as the most promising candidates for next-generation light-to-electricity technology. However, their practical application still suffers from energy loss induced by intrinsic defects within the perovskite lattice. Here, a refined defect passivation in perovskite films is designed, which shows a multi-interaction mechanism between the perovskite and passivator. Interestingly, a shift of molecular bonding is observed upon cooling down the film, leading to a stronger passivation of iodine/formamidine vacancies. Such mechanism on device under low-light and low-temperature conditions is further leveraged and a record efficiency over 45% with durable ambient stability (T90 > 4000 h) is obtained. The pioneer application of perovskite solar cells in above dual extreme conditions in this work reveals the key principles of designing functional groups for the passivators, and also demonstrates the capability of perovskites for diverse terrestrial energy conversion applications in demanding environments such as polar regions and outer space.

7.
Nat Commun ; 14(1): 839, 2023 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-36792606

RESUMEN

Even though the perovskite solar cell has been so popular for its skyrocketing power conversion efficiency, its further development is still roadblocked by its overall performance, in particular long-term stability, large-area fabrication and stable module efficiency. In essence, the soft component and ionic-electronic nature of metal halide perovskites usually chaperonage large number of anion vacancy defects that act as recombination centers to decrease both the photovoltaic efficiency and operational stability. Herein, we report a one-stone-for-two-birds strategy in which both anion-fixation and associated undercoordinated-Pb passivation are in situ achieved during crystallization by using a single amidino-based ligand, namely 3-amidinopyridine, for metal-halide perovskite to overcome above challenges. The resultant devices attain a power conversion efficiency as high as 25.3% (certified at 24.8%) with substantially improved stability. Moreover, the device without encapsulation retained 92% of its initial efficiency after 5000 h exposure in ambient and the device with encapsulation retained 95% of its initial efficiency after >500 h working at the maximum power point under continuous light irradiation in ambient. It is expected this one-stone-for-two-birds strategy will benefit large-area fabrication that desires for simplicity.

8.
Adv Mater ; 35(44): e2304809, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37669571

RESUMEN

The efficiency of metal halide perovskite solar cells (PSCs) has skyrocketed; however, defects created by aging precursor solutions and during crystallization pose a significant barrier to the reproducibility and efficiency of solar cells. In this work, fluoro-N,N,N″,N″-tetramethylformamidinium hexafluorophosphate (F-(CH3 )4 CN2 PF6 , abbreviated as TFFH) is introduced to stabilize precursor solution and improve crystallization dynamics simultaneously for high-performance formamidinium lead iodide (FAPbI3 )-based perovskite indoor photovoltaics. The TFFH stabilizes the precursor solution by inhibiting oxidation of I- and reducing newly generated I0 to I- , and passivates undercoordinated Pb2+ by interacting with the Pb─I framework. Time-resolved optical diagnostics show prolonged perovskite crystallization dynamics and in situ defect passivation due to the presence of strong FA+ ···TFFH···Pb─I interaction. Simultaneous regulation of precursor solution and crystallization dynamics guarantee larger perovskite grain sizes, better crystal orientation, fewer defects and more efficient charge extraction in PSCs. The optimized PSCs achieve improved reproducibility and better stability and reach an efficiency of 42.43% at illumination of 1002 lux, which is the highest efficiency among all indoor photovoltaics. It is anticipated that the concurrent stabilization of solutions and regulation of crystallization dynamics will emerge as a prevalent approach for enhancing the reproducibility and efficiency of perovskite.

9.
Adv Mater ; 35(42): e2305314, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37652150

RESUMEN

Understanding and controlling crystallization is crucial for high-quality perovskite films and efficient solar cells. Herein, the issue of defects in formamidinium lead iodide (FAPbI3 ) formation is addressed, focusing on the role of intermediates. A comprehensive picture of structural and carrier evolution during crystallization is demonstrated using in situ grazing-incidence wide-angle X-ray scattering, ultraviolet-visible spectroscopy and photoluminescence spectroscopy. Three crystallization stages are identified: precursors to the δ-FAPbI3 intermediate, then to α-FAPbI3 , where defects spontaneously emerge. A hydrogen-sulfate-based ionic liquid additive is found to enable the phase-conversion pathway of precursors → solvated intermediates → α-FAPbI3 , during which the spontaneous generation of δ-FAPbI3 can be effectively circumvented. This additive extends the initial growth kinetics and facilitates solvent-FA+ ion exchange, which results in the self-elimination of defects during crystallization. Therefore, the improved crystallization dynamics lead to larger grain sizes and fewer defects within thin films. Ultimately, the improved perovskite crystallization dynamics enable high-performance solar cells, achieving impressive efficiencies of 25.14% at 300 K and 26.12% at 240 K. This breakthrough might open up a new era of application for the emerging perovskite photovoltaic technology to low-temperature environments such as near-space and polar regions.

10.
Adv Mater ; 35(51): e2303384, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37572021

RESUMEN

Upscalable printing of high-performance and stable perovskite solar cells (PSCs) is highly desired for commercialization. However, the efficiencies of printed PSCs lag behind those of their lab-scale spin-coated counterparts owing to the lack of systematic understanding and control over perovskite crystallization dynamics. Here, the controlled crystallization dynamics achieved using an additive 1-butylpyridine tetrafluoroborate (BPyBF4 ) for high-quality ambient printed α-formamidinium lead triiodide (FAPbI3 ) perovskite films are reported. Using in situ grazing-incidence wide-angle X-ray scattering and optical diagnostics, the spontaneous formation of α-FAPbI3 from precursors during printing without the involvement of  Î´-FAPbI3 is demonstrated. The addition of BPyBF4 delays the crystallization onset of α-FAPbI3 , enhances the conversion from sol-gel to perovskite, and reduces stacking defects during printing. Therefore, the altered crystallization results in fewer voids, larger grains, and less trap-induced recombination loss within printed films. The printed PSCs yield high power conversion efficiencies of 23.50% and 21.60% for a 0.09 cm-2 area device and a 5 cm × 5 cm-area module, respectively. Improved device stability is further demonstrated, i.e., approximately 94% of the initial efficiency is retained for over 2400 h under ambient conditions without encapsulation. This study provides an effective crystallization control method for the ambient printing manufacture of large-area high-performance PSCs.

11.
Adv Mater ; 35(5): e2206451, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36427296

RESUMEN

Manipulating the formation process of the 2D/3D perovskite heterostructure, including its nucleation/growth dynamics and phase transition pathway, plays a critical role in controlling the charge transport between 2D and 3D crystals, and consequently, the scalable fabrication of efficient and stable perovskite solar cells. Herein, the structural evolution and phase transition pathways of the ligand-dependent 2D perovskite atop the 3D surface are revealed using time-resolved X-ray scattering. The results show that the ligand size and shape have a critical influence on the final 2D structure. In particular, ligands with smaller sizes and more reactive sites tend to form the n = 1 phase. Increasing the ligand size and decreasing the reactive sites promote the transformation from 3D to n = 3 and n < 3 phases. These findings are useful for the rational design of the phase distribution in 2D perovskites to balance the charge transport and stability of the perovskite films. Finally, solar cells based on ambient-printed CsPbI3 with n-butylammonium iodide treatment achieve an improved efficiency of 20.33%, which is the highest reported value for printed inorganic perovskite solar cells.

12.
Adv Mater ; 35(31): e2301140, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-36972593

RESUMEN

Surface-defect-triggered non-radiative charge recombination and poor stability have become the main roadblock to continued improvement in inorganic perovskite solar cells (PSCs). Herein, the main culprits are identified on the inorganic perovskite surface by first-principles calculations, and to purposefully design a brand-new passivator, Boc-S-4-methoxy-benzyl-l-cysteine (BMBC), whose multiple Lewis-based functional groups (NH, S and CO) to suppress halide vacancies and coordinate with undercoordinated Pb2+ through typical Lewis baseacid reactions. The tailored electron-donating methoxyl group (CH3 O-) can cause an increased electron density on the benzene ring, which strengthens the interaction with undercoordinated Pb2+ via electrostatic interactions. This BMBC passivation can reduce the surface trap density, enlarge grains, prolong the charge lifetime, and cause a more suitable energy-level alignment. In addition, the hydrophobic tert-butyl in butoxycarbonyl (Boc-) group ensures that BMBC is uniformly covered and prevents harmful aggregation through steric repulsion at the perovskite/hole-transporting layer (HTL) interface, thus providing a hydrophobic umbrella to resist moisture invasion. Consequently, the combination of the above increases the efficiency of CsPbI3-x Brx PSC from 18.6% to 21.8%, the highest efficiency for this type of inorganic metal halide PSCs so far, as far as it is known. Moreover, the device exhibits higher environmental and thermal stability.

13.
Adv Mater ; 34(10): e2106750, 2022 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-34964993

RESUMEN

All-inorganic cesium lead triiodide (CsPbI3 ) perovskite is well known for its unparalleled stability at high temperatures up to 500 °C and under oxidative chemical stresses. However, upscaling solar cells via ambient printing suffers from imperfect crystal quality and defects caused by uncontrollable crystallization. Here, the incorporation of a low concentration of novel ionic liquid is reported as being promising for managing defects in CsPbI3 films, interfacial energy alignment, and device stability of solar cells fabricated via ambient blade-coating. Both theoretical simulations and experimental measurements reveal that the ionic liquid successfully regulates the perovskite thin-film growth to decrease perovskite grain boundaries, strongly coordinates with the undercoordinated Pb2+ to passivate iodide vacancy defects, aligns the interface to decrease the energy barrier at the electron-transporting layer, and relaxes the lattice strain to promote phase stability. Consequently, ambient printed CsPbI3 solar cells with power conversion efficiency as high as 20.01% under 1 sun illumination (100 mW cm-2 ) and 37.24% under indoor light illumination (1000 lux, 365 µW cm-2 ) are achieved; both are the highest for printed all-inorganic cells for corresponding applications. Furthermore, the bare cells show an impressive long-term ambient stability with only ≈5% PCE degradation after 1000 h aging under ambient conditions.

14.
PLoS One ; 16(11): e0258962, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-34793463

RESUMEN

BACKGROUND: Tibial Pilon fractures are severe fractures accompanied by soft tissue injury. Although open reduction and internal fixation (ORIF) are effective in treating Pilon fractures, there is a controversy over time to surgery due to reported postoperative complications. However, there is no systematic review evaluating the difference of postoperative complications between early and delayed ORIF for treating pilon fractures. METHODS: Relevant literature written in English will be searched through PubMed, Cochrane Library, Embase, MEDLINE, and Web of Science. The study aims to compare the effects and complications of early and delayed ORIF for treating fresh pilon fractures in adult patients. The primary outcome will be infection rate, fracture union time, nonunion and malunion rate. And the secondary outcome will be metalwork removal, amputation, and ankle function grade. Two reviewers will independently assess the eligibility of the studies according to the pre-defined inclusion and exclusion criteria. A meta-analysis for the available data will be conducted using Revman 5.3. To measure effect size, odds ratios (ORs) and mean difference will be used for dichotomous and continuous data, respectively. Statistical heterogeneity will be explored. And a random-effects model or a fixed-effects will be used in pooled data on the basis of the existence or absence of heterogeneity. Subgroup analysis will be conducted to identify sources of heterogeneity and sensitivity analysis to test the results' robustness. We will assess the risk of bias by four different quality assessment tools according to the study design. Publication bias will be evaluated by funnel plot. The study data will be stored in the Open Science Framework website. PROSPERO REGISTRATION NUMBER: CRD42020207465.


Asunto(s)
Fijación Interna de Fracturas , Reducción Abierta , Traumatismos de los Tejidos Blandos , Fracturas de la Tibia , Humanos , Fracturas de Tobillo/fisiopatología , Fracturas de Tobillo/cirugía , Fijación Interna de Fracturas/métodos , Reducción Abierta/métodos , Complicaciones Posoperatorias/fisiopatología , Complicaciones Posoperatorias/terapia , Traumatismos de los Tejidos Blandos/fisiopatología , Traumatismos de los Tejidos Blandos/cirugía , Fracturas de la Tibia/fisiopatología , Fracturas de la Tibia/cirugía , Resultado del Tratamiento , Revisiones Sistemáticas como Asunto , Metaanálisis como Asunto
15.
Medicine (Baltimore) ; 99(9): e19211, 2020 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-32118722

RESUMEN

BACKGROUND: To assess the efficacy and safety of plaster splint vs splints in the treatment of distal radius fractures (DRFs). METHODS: For a more comprehensive collection of original study, we mainly searched 9 electronic databases including the PubMed, Web of Science, EMBASE, Cochrane Library, Cochrane Central Register of Controlled Trials (CENTRAL), Clinical Trials.gov, the Chinese National Knowledge Infrastructure Database (CNKI), Wanfang Database, and VIP Database. The retrieval date of all databases is from the establishment to January 2019. In the aspect of assessing the quality of original research methodology, we mainly rely on the Cochrane risk bias assessment tool and GRADE assessment method. Revman 5.3 is used for statistical analysis. RESULTS: A total of 8 studies involving 717 participants were included. The results showed that effective rate (RR = 0.99, 95%CI 0.91 to 1.07, P = .83), reduction rate (RR = 1.00, 95%CI 0.93 to 1.07, P = .98), and complication rate of the plaster splint had no significant difference with the splint. In addition, for the excellent rate of treatment, subgroup analysis based on the included studies found that when the intervention period was 4 weeks, the plaster splint was better than the splint, and when the intervention period was more than 4 weeks, there was no significant difference between them. CONCLUSIONS: There is no sufficient evidence that plaster splint is superior to splint. However, according to current evidence, plaster splint is more effective than splint when the intervention period is shorter (4 weeks), and its advantage disappears when the intervention period is longer (> 4 weeks). It should be noted that the results of this study were influenced by the sample size and the quality of the included studies. More high-quality and well-controlled RCTs are needed to draw better conclusions in further study.


Asunto(s)
Fracturas del Radio/terapia , Férulas (Fijadores) , Humanos , Ensayos Clínicos Controlados Aleatorios como Asunto , Resultado del Tratamiento
16.
Medicine (Baltimore) ; 98(31): e16562, 2019 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-31374022

RESUMEN

BACKGROUND: Distal radius fractures (DRFs) is one of the most common bone injuries in children, which may lead to deformity and other complications if the treatment is not prompt or appropriate. Splints external fixation is a common conservative treatment for such fractures. Therefore, we conducted a systematic review and meta-analysis to explore the efficacy, safety and cost benefits of splints in the treatment of DRFs in children. METHODS: PubMed, Web of Science, Embase, Cochrane Library, Cochrane Central Register of Controlled Trials (CENTRAL), and ClinicalTrials.gov, Chinese National Knowledge Infrastructure Database (CNKI), Wanfang Database, and VIP Database were searched for eligible randomized controlled trials (RCTs). The methodological quality of the included studies and the level of evidence for results were assessed, respectively, using the risk bias assessment tool of Cochrane and the Grading of Recommendations Assessment, Development, and Evaluation (GRADE) method. Statistical analysis was conducted with Revman 5.3. RESULTS: This study will analyze and integrate the existing evidence for effectiveness, safety and cost benefits of splints on DRFs in children. CONCLUSION: The conclusion of this study will provide evidence to effectiveness, safety and cost benefits of splints on DRFs in children, which can further guide the selection of appropriate interventions. PROSPERO REGISTRATION NUMBER: CRD42019123429.


Asunto(s)
Fracturas del Radio , Férulas (Fijadores) , Adolescente , Niño , Preescolar , Humanos , Seguridad del Paciente/normas , Pediatría/instrumentación , Pediatría/métodos , Fracturas del Radio/economía , Fracturas del Radio/terapia , Férulas (Fijadores)/efectos adversos , Férulas (Fijadores)/economía , Férulas (Fijadores)/normas , Metaanálisis como Asunto , Revisiones Sistemáticas como Asunto
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