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1.
Nature ; 609(7926): 369-374, 2022 09.
Artículo en Inglés | MEDLINE | ID: mdl-36045296

RESUMEN

Recently, chimeric antigen receptor (CAR)-T cell therapy has shown great promise in treating haematological malignancies1-7. However, CAR-T cell therapy currently has several limitations8-12. Here we successfully developed a two-in-one approach to generate non-viral, gene-specific targeted CAR-T cells through CRISPR-Cas9. Using the optimized protocol, we demonstrated feasibility in a preclinical study by inserting an anti-CD19 CAR cassette into the AAVS1 safe-harbour locus. Furthermore, an innovative type of anti-CD19 CAR-T cell with PD1 integration was developed and showed superior ability to eradicate tumour cells in xenograft models. In adoptive therapy for relapsed/refractory aggressive B cell non-Hodgkin lymphoma (ClinicalTrials.gov, NCT04213469 ), we observed a high rate (87.5%) of complete remission and durable responses without serious adverse events in eight patients. Notably, these enhanced CAR-T cells were effective even at a low infusion dose and with a low percentage of CAR+ cells. Single-cell analysis showed that the electroporation method resulted in a high percentage of memory T cells in infusion products, and PD1 interference enhanced anti-tumour immune functions, further validating the advantages of non-viral, PD1-integrated CAR-T cells. Collectively, our results demonstrate the high safety and efficacy of non-viral, gene-specific integrated CAR-T cells, thus providing an innovative technology for CAR-T cell therapy.


Asunto(s)
Inmunoterapia Adoptiva , Linfoma de Células B , Receptores Quiméricos de Antígenos , Animales , Antígenos CD19/inmunología , Electroporación , Humanos , Inmunoterapia Adoptiva/efectos adversos , Inmunoterapia Adoptiva/métodos , Linfoma de Células B/inmunología , Linfoma de Células B/patología , Linfoma de Células B/terapia , Células T de Memoria/inmunología , Receptor de Muerte Celular Programada 1/inmunología , Receptores Quiméricos de Antígenos/inmunología , Receptores Quiméricos de Antígenos/uso terapéutico , Recurrencia , Análisis de la Célula Individual , Ensayos Antitumor por Modelo de Xenoinjerto
2.
J Virol ; 98(7): e0075324, 2024 Jul 23.
Artículo en Inglés | MEDLINE | ID: mdl-38829136

RESUMEN

Porcine hemagglutinating encephalomyelitis virus (PHEV), a neurotropic betacoronavirus, is prevalent in natural reservoir pigs and infects mice. This raises concerns about host jumping or spillover, but little is known about the cause of occurrence. Here, we revealed that dipeptidyl peptidase 4 (DPP4) is a candidate binding target of PHEV spikes and works as a broad barrier to overcome. Investigations of the host breadth of PHEV confirmed that cells derived from pigs and mice are permissive to virus propagation. Both porcine DPP4 and murine DPP4 have high affinity for the viral spike receptor-binding domain (RBD), independent of their catalytic activity. Loss of DPP4 expression results in limited PHEV infection. Structurally, PHEV spike protein binds to the outer surface of blades IV and V of the DPP4 ß-propeller domain, and the DPP4 residues N229 and N321 (relative to human DPP4 numbering) participate in RBD binding via its linked carbohydrate entities. Removal of these N-glycosylations profoundly enhanced the RBD-DPP4 interaction and viral invasion, suggesting they act as shielding in PHEV infection. Furthermore, we found that glycosylation, rather than structural differences or surface charges, is more responsible for DPP4 recognition and species barrier formation. Overall, our findings shed light on virus-receptor interactions and highlight that PHEV tolerance to DPP4 orthologs is a putative determinant of its cross-species transmission or host range expansion.IMPORTANCEPHEV is a neurotropic betacoronavirus that is circulating worldwide and has raised veterinary and economic concerns. In addition to being a reservoir species of pigs, PHEV can also infect wild-type mice, suggesting a "host jump" event. Understanding cross-species transmission is crucial for disease prevention and control but remains to be addressed. Herein, we show that the multifunctional receptor DPP4 plays a pivotal role in the host tropism of PHEV and identifies the conserved glycosylation sites in DPP4 responsible for this restriction. These findings highlight that the ability of PHEV to utilize DPP4 orthologs potentially affects its natural host expansion.


Asunto(s)
Dipeptidil Peptidasa 4 , Especificidad del Huésped , Glicoproteína de la Espiga del Coronavirus , Animales , Dipeptidil Peptidasa 4/metabolismo , Dipeptidil Peptidasa 4/genética , Porcinos , Ratones , Glicoproteína de la Espiga del Coronavirus/metabolismo , Glicoproteína de la Espiga del Coronavirus/genética , Glicoproteína de la Espiga del Coronavirus/química , Humanos , Unión Proteica , Infecciones por Coronavirus/virología , Infecciones por Coronavirus/veterinaria , Infecciones por Coronavirus/metabolismo , Infecciones por Coronavirus/transmisión , Enfermedades de los Porcinos/virología , Glicosilación , Internalización del Virus , Línea Celular , Betacoronavirus 1/metabolismo , Células HEK293 , Deltacoronavirus
3.
Nano Lett ; 24(1): 441-449, 2024 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-38109494

RESUMEN

Conjugated polymer films are promising in wearable X-ray detection. However, achieving optimal film microstructure possessing good electrical and detection performance under large deformation via scalable printing remains challenging. Herein, we report bar-coated high-performance stretchable films based on a conjugated polymer P(TDPP-Se) and elastomer SEBS blend by optimizing the solution-processing conditions. The moderate preaggregation in solution and prolonged growth dynamics from a solvent mixture with limited dissolving capacity is critical to forming aligned P(TDPP-Se) chains/crystalline nanofibers in the SEBS phase with enhanced π-π stacking for charge transport and stress dissipation. The film shows a large elongation at break of >400% and high mobilities of 5.29 cm2 V-1 s-1 at 0% strain and 1.66 cm2 V-1 s-1 over 500 stretch-release cycles at 50% strain, enabling good X-ray imaging with a high sensitivity of 1501.52 µC Gyair-1 cm-2. Our work provides a morphology control strategy toward high-performance conjugated polymer film-based stretchable electronics.

4.
Small ; : e2403566, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38949415

RESUMEN

Amidino-based additives show great potential in high-performance perovskite solar cells (PSCs). However, the role of different functional groups in amidino-based additives have not been well elucidated. Herein, two multifunctional amidino additives 4-amidinobenzoic acid hydrochloride (ABAc) and 4-amidinobenzamide hydrochloride (ABAm) are employed to improve the film quality of formamidinium lead iodide (FAPbI3) perovskites. Compared with ABAc, the amide group imparts ABAm with larger dipole moment and thus stronger interactions with the perovskite components, i.e., the hydrogen bonds between N…H and I- anion and coordination bonds between C = O and Pb2+ cation. It strengthens the passivation effect of iodine vacancy defect and slows down the crystallization process of α-FAPbI3, resulting in the significantly reduced non-radiative recombination, long carrier lifetime of 1.7 µs, uniformly large crystalline grains, and enhances hydrophobicity. Profiting from the improved film quality, the ABAm-treated PSC achieves a high efficiency of 24.60%, and maintains 93% of the initial efficiency after storage in ambient environment for 1200 hours. This work provides new insights for rational design of multifunctional additives regarding of defect passivation and crystallization control toward highly efficient and stable PSCs.

5.
Small ; 20(13): e2308945, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-37948432

RESUMEN

The family of metal-free molecular perovskites, an emerging novel class of eco-friendly semiconductor, welcomes a new member with a unique 1D hexagonal perovskite structure. Lowering dimensionality at molecular level is a facile strategy for crystal structure conversion, optoelectronic property regulation, and device performance optimization. Herein, the study reports the design, synthesis, packing structure, and photophysical properties of the 1D metal-free molecular perovskite-related single crystal, rac-3APD-NH4I3(rac-3APD= racemic-3-Aminopiperidinium), that features a quantum wire structure formed by infinite chains of face-sharing NH4I6 octahedra, enabling strong quantum confinement with strongly self-trapped excited (STE) states to give efficient warm orange emission with a photoluminescence quantum yield (PLQY) as high as ≈41.6%. The study accordingly unveils its photoexcited carrier dynamics: rac-3APD-NH4I3 relaxes to STE state with a short lifetime of 10 ps but decays to ground state by emitting photons with a relatively longer lifetime of 560 ps. Additionally, strong quantum confinement effect is conducive to charge transport along the octahedral channels that enables the co-planar single-crystal X-ray detectors to achieve a sensitivity as high as 1556 µC Gyair -1 cm-2. This work demonstrates the first case of photoluminescence mechanism and photophysical dynamics of 1D metal-free perovskite-related semiconductor, as well as the promise for high-performance X-ray detector.

6.
Small ; : e2401701, 2024 May 05.
Artículo en Inglés | MEDLINE | ID: mdl-38705844

RESUMEN

Enhancing the intrinsic stability of perovskite and through encapsulation to isolate water, oxygen, and UV-induced decomposition are currently common and most effective strategies in perovskite solar cells. Here, the atomic layer deposition process is employed to deposit a nanoscale (≈100 nm), uniform, and dense Al2O3 film on the front side of perovskite devices, effectively isolating them from the erosion caused by water and oxygen in the humid air. Simultaneously, nanoscale (≈100 nm) TiO2 films are also deposited on the glass surface to efficiently filter out the ultraviolet (UV) light in the light source, which induces degradation in perovskite. Ultimately, throughthe collaborative effects of both aspects, the stability of the devices is significantly improved under conditions of humid air and illumination. As a result, after storing the devices in ambient air for 1000 h, the efficiency only declines to 95%, and even after 662 h of UV exposure, the efficiency remains at 88%, far surpassing the performance of comparison devices. These results strongly indicate that the adopted Al2O3 and TiO2 thin films play a significant role in enhancing the stability of perovskite solar cells, demonstrating substantial potential for widespread industrial applications.

7.
J Virol ; 97(12): e0133823, 2023 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-38009916

RESUMEN

IMPORTANCE: Betacoronaviruses, including severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) and mouse hepatitis virus (MHV), exploit the lysosomal exocytosis pathway for egress. However, whether all betacoronaviruses members use the same pathway to exit cells remains unknown. Here, we demonstrated that porcine hemagglutinating encephalomyelitis virus (PHEV) egress occurs by Arl8b-dependent lysosomal exocytosis, a cellular egress mechanism shared by SARS-CoV-2 and MHV. Notably, PHEV acidifies lysosomes and activates lysosomal degradative enzymes, while SARS-CoV-2 and MHV deacidify lysosomes and limit the activation of lysosomal degradative enzymes. In addition, PHEV release depends on V-ATPase-mediated lysosomal pH. Furthermore, this is the first study to evaluate ßCoV using lysosome for spreading through the body, and we have found that lysosome played a critical role in PHEV neural transmission and brain damage caused by virus infection in the central nervous system. Taken together, different betacoronaviruses could disrupt lysosomal function differently to exit cells.


Asunto(s)
Betacoronavirus 1 , Infecciones por Coronavirus , Exocitosis , Lisosomas , Neuronas , Animales , Ratones , Betacoronavirus 1/metabolismo , Lisosomas/enzimología , Lisosomas/metabolismo , Lisosomas/virología , Virus de la Hepatitis Murina/metabolismo , Neuronas/enzimología , Neuronas/metabolismo , Neuronas/patología , Neuronas/virología , SARS-CoV-2/metabolismo , Porcinos/virología , Concentración de Iones de Hidrógeno , ATPasas de Translocación de Protón Vacuolares/metabolismo , Infecciones por Coronavirus/patología , Infecciones por Coronavirus/transmisión , Infecciones por Coronavirus/virología
8.
PLoS Pathog ; 18(6): e1010667, 2022 06.
Artículo en Inglés | MEDLINE | ID: mdl-35759516

RESUMEN

Porcine hemagglutinating encephalomyelitis virus (PHEV) is a highly neurotropic coronavirus belonging to the genus Betacoronavirus. Similar to pathogenic coronaviruses to which humans are susceptible, such as SARS-CoV-2, PHEV is transmitted primarily through respiratory droplets and close contact, entering the central nervous system (CNS) from the peripheral nerves at the site of initial infection. However, the neuroinvasion route of PHEV are poorly understood. Here, we found that BALB/c mice are susceptible to intranasal PHEV infection and showed distinct neurological manifestations. The behavioral study and histopathological examination revealed that PHEV attacks neurons in the CNS and causes significant smell and taste dysfunction in mice. By tracking neuroinvasion, we identified that PHEV invades the CNS via the olfactory nerve and trigeminal nerve located in the nasal cavity, and olfactory sensory neurons (OSNs) were susceptible to viral infection. Immunofluorescence staining and ultrastructural observations revealed that viral materials traveling along axons, suggesting axonal transport may engage in rapid viral transmission in the CNS. Moreover, viral replication in the olfactory system and CNS is associated with inflammatory and immune responses, tissue disorganization and dysfunction. Overall, we proposed that PHEV may serve as a potential prototype for elucidating the pathogenesis of coronavirus-associated neurological complications and olfactory and taste disorders.


Asunto(s)
Betacoronavirus 1 , COVID-19 , Infecciones por Coronavirus/patología , Trastornos del Olfato , Animales , Betacoronavirus 1/fisiología , Humanos , Ratones , Trastornos del Olfato/virología , SARS-CoV-2 , Olfato , Porcinos
9.
Respir Res ; 25(1): 132, 2024 Mar 18.
Artículo en Inglés | MEDLINE | ID: mdl-38500137

RESUMEN

OBJECTIVES: Non-tuberculous mycobacteria (NTM) infection is an increasing health problem due to delaying an effective treatment. However, there are few data on 18F-FDG PET/CT for evaluating the status of NTM patients. The aim of this study was to investigate the potential value of 18F-FDG PET/CT in guiding the treatment strategy of NTM patients. METHODS: We retrospectively analyzed the cases of 23 NTM patients who underwent 18F-FDG PET/CT. The clinical data, including immune status and severity of NTM pulmonary disease (NTM-PD), were reviewed. The metabolic parameters of 18F-FDG included maximum standardized uptake value (SUVmax), SUVmax of the most FDG-avid lesion (SUVTop), SUVTop/SUVmax of the liver (SURLiver), SUVTop/SUVmax of the blood (SURBlood), metabolic lesion volume (MLV), and total lesion glycolysis (TLG). The optimal cut-off values of these parameters were determined using receiver operating characteristic curves. RESULTS: There were 6 patients (26.09%) with localized pulmonary diseases and 17 patients (73.91%) with disseminated diseases. The NTM lesions had high or moderate 18F-FDG uptake (median SUVTop: 8.2 ± 5.7). As for immune status, the median SUVTop in immunocompromised and immunocompetent patients were 5.2 ± 2.5 and 10.0 ± 6.4, respectively, with a significant difference (P = 0.038). As for extent of lesion involvement, SURLiver and SURBlood in localized pulmonary and disseminated diseases were 1.9 ± 1.1 vs. 3.8 ± 1.6, and 2.7 ± 1.8 vs. 5.5 ± 2.6, respectively, with a significant difference (P = 0.016 and 0.026). Moreover, for disease severity, SUVmax of the lung lesion (SUVI-lung) and SUVmax of the marrow (SUVMarrow) in the severe group were 7.7 ± 4.3 and 4.4 ± 2.7, respectively, significantly higher than those in the non-severe group (4.4 ± 2.0 and 2.4 ± 0.8, respectively) (P = 0.027 and 0.036). The ROC curves showed that SUVTop, SURLiver, SURBlood, SUVI-lung, and SUVMarrow had a high sensitivity and specificity for the identification of immune status, lesion extent, and severity of disease in NTM patients. CONCLUSION: 18F-FDG PET/CT is a useful tool in the diagnosis, evaluation of disease activity, immune status, and extent of lesion involvement in NTM patients, and can contribute to planning the appropriate treatment for NTM.


Asunto(s)
Fluorodesoxiglucosa F18 , Tomografía Computarizada por Tomografía de Emisión de Positrones , Humanos , Tomografía Computarizada por Tomografía de Emisión de Positrones/métodos , Estudios Retrospectivos , Tomografía de Emisión de Positrones , Curva ROC
10.
Eur J Nucl Med Mol Imaging ; 51(9): 2806-2818, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38691111

RESUMEN

PURPOSE: Biochemical recurrence (BCR) following radical prostatectomy (RP) is a significant concern for patients with prostate cancer. Reliable prediction models are needed to identify patients at risk for BCR and facilitate appropriate management. This study aimed to develop and validate a clinical-radiomics model based on preoperative [18 F]PSMA-1007 PET for predicting BCR-free survival (BRFS) in patients who underwent RP for prostate cancer. MATERIALS AND METHODS: A total of 236 patients with histologically confirmed prostate cancer who underwent RP were retrospectively analyzed. All patients had a preoperative [18 F]PSMA-1007 PET/CT scan. Radiomics features were extracted from the primary tumor region on PET images. A radiomics signature was developed using the least absolute shrinkage and selection operator (LASSO) Cox regression model. The performance of the radiomics signature in predicting BRFS was assessed using Harrell's concordance index (C-index). The clinical-radiomics nomogram was constructed using the radiomics signature and clinical features. The model was externally validated in an independent cohort of 98 patients. RESULTS: The radiomics signature comprised three features and demonstrated a C-index of 0.76 (95% CI: 0.60-0.91) in the training cohort and 0.71 (95% CI: 0.63-0.79) in the validation cohort. The radiomics signature remained an independent predictor of BRFS in multivariable analysis (HR: 2.48, 95% CI: 1.47-4.17, p < 0.001). The clinical-radiomics nomogram significantly improved the prediction performance (C-index: 0.81, 95% CI: 0.66-0.95, p = 0.007) in the training cohort and (C-index: 0.78 95% CI: 0.63-0.89, p < 0.001) in the validation cohort. CONCLUSION: We developed and validated a novel [18 F]PSMA-1007 PET-based clinical-radiomics model that can predict BRFS following RP in prostate cancer patients. This model may be useful in identifying patients with a higher risk of BCR, thus enabling personalized risk stratification and tailored management strategies.


Asunto(s)
Tomografía Computarizada por Tomografía de Emisión de Positrones , Prostatectomía , Neoplasias de la Próstata , Humanos , Masculino , Neoplasias de la Próstata/diagnóstico por imagen , Neoplasias de la Próstata/cirugía , Persona de Mediana Edad , Anciano , Estudios Retrospectivos , Oligopéptidos/química , Supervivencia sin Enfermedad , Procesamiento de Imagen Asistido por Computador , Radiómica , Niacinamida/análogos & derivados
11.
Clin Transplant ; 38(4): e15300, 2024 04.
Artículo en Inglés | MEDLINE | ID: mdl-38555576

RESUMEN

Cytomegalovirus (CMV) reactivation remains one of the major and life-threatening complications after allogeneic hematopoietic stem cell transplantation (allo-HSCT). Yet, there is still a lack of safe and effective ways to prevent CMV reactivation in allo-HSCT patients. Here, we retrospectively analyzed a cohort of patients who underwent HSCT at our transplant center between 2018 and 2022 to evaluate the efficacy of prophylactic CMV-specific intravenous immunoglobulin (CMV-IVIg) against CMV reactivation. After Propensity Score Matching, the CMV reactivation rate was significantly decreased in the CMV-IVIg group (HR, 2.952; 95% CI,1.492-5.841; P = .002) compared with the control group. Additionally, the time duration of CMV reactivation (P = .001) and bacterial infection rate (P = .013) were significantly lower in the CMV-IVIg group. Moreover, prophylactic CMV-IVIg was more effective in CMV seropositive patients who received ATG as part of GVHD prevention (HR, 8.225; 95% CI,1.809-37.39; P = .006). In conclusion, CMV-IVIg is considered an effective and safe way to prevent CMV reactivation in HSCT recipients, which may be related to the acceleration of immune reconstitution in the early stage after transplantation.


Asunto(s)
Infecciones por Citomegalovirus , Trasplante de Células Madre Hematopoyéticas , Humanos , Citomegalovirus , Inmunoglobulinas Intravenosas/uso terapéutico , Infecciones por Citomegalovirus/etiología , Infecciones por Citomegalovirus/prevención & control , Infecciones por Citomegalovirus/tratamiento farmacológico , Estudios Retrospectivos , Trasplante Homólogo , Trasplante de Células Madre Hematopoyéticas/efectos adversos , Anticuerpos Antivirales
12.
Macromol Rapid Commun ; 45(1): e2300240, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37289949

RESUMEN

The physical blending of high-mobility conjugated polymers with ductile elastomers provides a simple way to realize high-performance stretchable films. However, how to control the morphology of the conjugated polymer and elastomer blend film and its response to mechanical fracture processes during stretching are not well understood. Herein, a sandwich structure is constructed in the blend film based on a conjugated polymer poly[(5-fluoro-2,1,3-benzothiadiazole-4,7-diyl)(4,4-dihexadecyl-4H-cyclopenta[2,1-b:3,4-b″]dithiophene-2,6-diyl)(6-fluoro-2,1,3-benzothiadiazole-4,7-diyl)(4,4-dihexadecyl-4H-cyclopenta[2,1-b:3,4-b″]dithiophene-2,6-diyl)] (PCDTFBT) and an elastomer polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene (SEBS). The sandwich structure is composed of a PCDTFBT:SEBS mixed layer laminated with a PCDTFBT-rich layer at both the top and bottom surfaces. During stretching, the external strain energy can be effectively dissipated by the deformation of the crystalline PCDTFBT domains and amorphous SEBS phases and the recrystallization of the PCDTFBT chains. This endows the blend film with excellent ductility, with a large crack onset strain exceeding 1100%, and minimized the electrical degradation of the blend film at a large strain. This study indicates that the electrical and mechanical performance of conjugated polymer/elastomer blend films can be improved by manipulating their microstructure.


Asunto(s)
Polímeros , Tiadiazoles , Elastómeros/química , Polímeros/química , Poliestirenos , Tiadiazoles/química , Tiofenos/química
13.
Angew Chem Int Ed Engl ; 63(17): e202400205, 2024 Apr 22.
Artículo en Inglés | MEDLINE | ID: mdl-38436587

RESUMEN

The perovskite/silicon tandem solar cell (TSC) has attracted tremendous attention due to its potential to breakthrough the theoretical efficiency set for single-junction solar cells. However, the perovskite solar cell (PSC) designed as its top component cell suffers from severe photo-induced halide segregation owing to its mixed-halide strategy for achieving desirable wide-bandgap (1.68 eV). Developing pure-iodide wide-bandgap perovskites is a promising route to fabricate photostable perovskite/silicon TSCs. Here, we report efficient and photostable pure-iodide wide-bandgap PSCs made from an anti-solvent-free (ASF) technique. The ASF process is achieved by mixing two precursor solutions, both of which are capable of depositing corresponding perovskite films without involving anti-solvent. The mixed solution finally forms Cs0.3DMA0.2MA0.5PbI3 perovskite film with a bandgap of 1.68 eV. Furthermore, methylammonium chloride additive is applied to enhance the crystallinity and reduce the trap density of perovskite films. As a result, the pure-iodide wide-bandgap PSC delivers efficiency as high as 21.30 % with excellent photostability, the highest for this type of solar cells. The ASF method significantly improves the device reproducibility as compared with devices made from other anti-solvent methods. Our findings provide a novel recipe to prepare efficient and photostable wide-bandgap PSCs.

14.
Angew Chem Int Ed Engl ; 63(30): e202404401, 2024 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-38729917

RESUMEN

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.

15.
Angew Chem Int Ed Engl ; 63(22): e202403739, 2024 May 27.
Artículo en Inglés | MEDLINE | ID: mdl-38565430

RESUMEN

Deep-blue perovskite light-emitting diodes (PeLEDs) based on quasi-two-dimensional (quasi-2D) systems exist heightened sensitivity to the domain distribution. The top-down crystallization mode will lead to a vertical gradient distribution of quantum well (QW) structure, which is unfavorable for deep-blue emission. Herein, a thermal gradient annealing treatment is proposed to address the polydispersity issue of vertical QWs in quasi-2D perovskites. The formation of large-n domains at the upper interface of the perovskite film can be effectively inhibited by introducing a low-temperature source in the annealing process. Combined with the utilization of NaBr to inhibit the undesirable n=1 domain, a vertically concentrated QW structure is ultimately attained. As a result, the fabricated device delivers a narrow and stable deep-blue emission at 458 nm with an impressive external quantum efficiency (EQE) of 5.82 %. Green and sky-blue PeLEDs with remarkable EQE of 21.83 % and 17.51 % are also successfully achieved, respectively, by using the same strategy. The findings provide a universal strategy across the entire quasi-2D perovskites, paving the way for future practical application of PeLEDs.

16.
Angew Chem Int Ed Engl ; 63(7): e202318133, 2024 Feb 12.
Artículo en Inglés | MEDLINE | ID: mdl-38168100

RESUMEN

Buried interface modification can effectively improve the compatibility between interfaces. Given the distinct interface selections in perovskite solar cells (PSCs), the applicability of a singular modification material remains limited. Consequently, in response to this challenge, we devised a tailored molecular strategy based on the electronic effects of specific functional groups. Therefore, we prepared three distinct silane coupling agents, and due to the varying inductive effects of these functional groups, the electronic distribution and molecular dipole moments of the coupling agents are correspondingly altered. Among them, trimethoxy (3,3,3-trifluoropropyl)-silane (F3 -TMOS), which possesses electron-withdrawing groups, generates a molecular dipole moment directed toward the hole transport layer (HTL). This approach changes the work function of the HTL, optimizes the energy level alignment, reduces the open-circuit voltage loss, and facilitates carrier transport. Furthermore, through the buffering effect of the coupling agent, the interface strain and lattice distortion caused by annealing the perovskite are reduced, enhancing the stability of the tin-based perovskite. Encouragingly, tin PSCs treated with F3 -TMOS achieved a champion efficiency of 14.67 %. This strategy provides an expedient avenue for the design of buried interface modification materials, enabling precise molecular adjustments in accordance with distinct interfacial contexts to ameliorate mismatched energetics and enhance carrier dynamics.

17.
Angew Chem Int Ed Engl ; : e202406140, 2024 Jul 09.
Artículo en Inglés | MEDLINE | ID: mdl-38981859

RESUMEN

Blue perovskite light-emitting diodes (PeLEDs) are crucial avenues for achieving full-color displays and lighting based on perovskite materials. However, the relatively low external quantum efficiency (EQE) has hindered their progression towards commercial applications. Quasi-two-dimensional (quasi-2D) perovskites stand out as promising candidates for blue PeLEDs, with optimized control over low-dimensional phases contributing to enhanced radiative properties of excitons. Herein, the impact of organic molecular dopants on the crystallization of various n-phase structures in quasi-2D perovskite films. The results reveal that the highly reactive bis(4-(trifluoromethyl)phenyl)phosphine oxide (BTF-PPO) molecule could effectively restrain the formation of organic spacer cation-ordered layered perovskite phases through chemical reactions, simultaneously passivate those uncoordinated Pb2+ defects. Consequently, the prepared PeLEDs exhibited a maximum EQE of 16.6% (@ 490 nm). The finding provides a new route to design dopant molecules for phase modulation in quasi-2D PeLEDs.

18.
Small ; 19(52): e2305064, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37635401

RESUMEN

Due to their greater opt electric performance, perovskite photovoltaics (PVs) present huge potential to be commercialized. Perovskite PV's high theoretical efficiency expands the available development area. The passivation of defects in perovskite films is crucial for approaching the theoretical limit. In addition to creating efficient passivation techniques, it is essential to direct the passivation approach by getting precise and real-time information on the trap states through measurements. Therefore, it is necessary to establish quantitative characterization methods for the trap states in energy and 3D spaces. The authors cover the characterization of the spatial and energy distributions of trap states in this article with an eye toward high-efficiency perovskite photovoltaics. After going over the strategies that have been created for characterizing and evaluating trap states, the authors will concentrate on how to direct the creative development of characterization techniques for trap states assessment and highlight the opportunities and challenges of future development. The 3D space and energy distribution mappings of trap states are anticipated to be realized. The review will give key guiding importance for further approaching the theoretical efficiency of perovskite photovoltaics, offering some future research direction and technological assistance for the development of appropriate targeted passivation technologies.

19.
Small ; 19(38): e2302585, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37196420

RESUMEN

Owing to the merits of low cost and high power conversion efficiency (PCE), perovskite solar cells (PSCs) have become the best candidate to replace the commonly used silicon solar cells. However, PSCs have been slow to enter the market for a number of reasons, including poor stability, high toxicity, and rigorous preparation process. Passivation strategies including surface passivation and bulk passivation have been successfully applied to improve the device performance of PSCs. The passivation of the defects at the buried interface, which is regarded as a key strategy to breakthrough the device efficiency and stability of PSCs in the future, is ongoing with challenge. Herein, in detail the recent passivation of the buried interface is introduced from three aspects: perovskite layer, buried interlayer, and transport layer. The passivation effect of the buried interface is clearly demonstrated through three categories of salts, organics, and 2D materials. In addition, the transport layer is classified into electron transport layer (ETL) and hole transport layer (HTL). These classifications can help to have a clear understanding of substances which generate passivating effect and guide the continuous promotion of the follow-up buried interface passivating work.

20.
Small ; 19(16): e2206581, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36670076

RESUMEN

Organic-inorganic halide perovskites (OIHPs) obtained tremendous attention due to their low cost and excellent properties. However, the stability and toxicity of Pb-based OIHPs (POIHPs), as well as the weakness of efficiency and stability in Sn-based OIHPs (SOIHPs), are still serious issues for commercial application. Notably, composition engineering is an effective and direct strategy for improving these issues along with the control and modification of properties. Recently, the doping strategies for POIHPs and SOIHPs are booming. Based on the relationship between properties and composition, the doping strategies for POIHPs and SOIHPs, aiming to provide a comprehensive review and guidance for the research are systematically summarized. Moreover, the doping strategies for Pb-Sn mixed OIHPs are also discussed. Finally, a brief perspective and conclusion toward future possible doping schemes and properties designment of POIHPs and SOIHPs are offered.

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