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FAPbI3 stands out as an ideal candidate for the photoabsorbing layer of perovskite solar cells (PSCs), showcasing outstanding photovoltaic properties. Nonetheless, stabilizing photoactive α-FAPbI3 remains a challenge due to the lower formation energy of the competitive photoinactive δ-phase. In this study, we employ tetraethylphosphonium lead tribromide (TEPPbBr3) single crystals as templates for the epitaxial growth of PbI2. The strategic use of TEPPbBr3 optimizes the evolution of intermediates and the crystallization kinetics of perovskites, leading to high-quality and phase-stable α-FAPbI3 films. The TEPPbBr3-modified perovskite exhibits optimized carrier dynamics, yielding a champion efficiency of 25.13% with a small voltage loss of 0.34 V. Furthermore, the target device maintains 90% of its initial PCE under maximum power point (MPP) tracking over 1000 h. This work establishes a promising pathway through single crystal seed based epitaxial growth for achieving satisfactory crystallization regulation and phase stabilization of α-FAPbI3 perovskites toward high-efficiency and stable PSCs.
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Oxygen-vacancy (Ov) engineering is an effective strategy to manipulate the electronic configuration of catalysts for electrochemical nitrogen reduction reaction (eNRR). The influence of the stable facet on the electronic configuration of Ov is widely studied, however, the effect of the reactive facet on the local electron density of Ov is unveiled. In this work, an eNRR electrode R(111)-TiO2/HGO is provided with a high proportion exposed reactive facet (111) of rutile-TiO2 (denoted as R(111)-TiO2) nanocrystals with Ov anchored in hierarchically porous graphite oxide (HGO) nanofilms. The R(111)-TiO2/HGO exhibits excellent eNRR performance with an NH3 yield rate of 20.68 µg h-1 cm-2, which is ≈20 times the control electrode with the most stable facet (110) exposed (R(110)-TiO2/HGO). The experimental data and theoretical simulations reveal that the crystal facet (111) has a positive effect on regulating the local electron density around the oxygen vacancy and the two adjacent Ti-sites, promoting the π-back-donation, minimizing the eNRR barrier, and transforming the rate determination step to *NNHâ*NNHH. This work illuminates the effect of crystal facet on the performance of eNRR, and offers a novel strategy to design efficient eNRR catalysts.
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OBJECTIVES: The aim of this study was to investigate the changes in various parameters of contrast-enhanced ultrasound (CEUS) before and after treatment in patients with IgG4-related autoimmune pancreatitis (IgG4-AIP), and to identify potential indicators that can assist in evaluating disease activity. METHODS: In this prospective study, we enrolled patients diagnosed with IgG4-AIP from June 2021 to November 2022. Demographic characteristics, clinical features, laboratory tests were recorded. Baseline and follow-up, conventional ultrasound and CEUS were conducted. Additionally, a region of interest (ROI) within lesions, pancreatic head, pancreatic body, and pancreatic tail was taken to draw time-intensity curves (TIC) and parameters of TIC were recorded and analysed. RESULTS: Seventy-three active IgG4-AIP patients were enrolled. Follow-up, a notable decrease in the size of the pancreatic lesion was observed with a reduction in the maximum diameter from 4.3 ± 2.0 cm to 1.7 ± 1.6 cm (p=0.01). The results revealed a statistically significant increase in peak intensity (PI) in the head, body, and tail regions of the pancreas (p<0.001), along with a significant rise in the area under the curve (AUC) in the tail region of the pancreas (p=0.029) after treatment compared to baseline. In contrast, no statistically significant differences were observed in other parameters of TIC. A significant increase of PI was observed in 12 patients with diffuse IgG4-AIP following treatment. Following treatment, there was a significant increase in PI in the focal area among the 12 patients with focal lesions. CONCLUSIONS: CEUS based on TIC holds great potential for assessing response to treatment in patients with IgG4 AIP.
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OBJECTIVE: To investigate the rates of low disease activity and clinical remission in patients with systemic lupus erythematosus (SLE) in a real-world setting, and to analyze the related factors of low disease activity and clinical remission. METHODS: One thousand patients with SLE were enrolled from 11 teaching hospitals. Demographic, clinical and laboratory data, as well as treatment regimes were collec-ted by self-completed questionnaire. The rates of low disease activity and remission were calculated based on the lupus low disease activity state (LLDAS) and definitions of remission in SLE (DORIS). Charac-teristics of patients with LLDAS and DORIS were analyzed. Multivariate Logistic regression analysis was used to evaluate the related factors of LLDAS and DORIS remission. RESULTS: 20.7% of patients met the criteria of LLDAS, while 10.4% of patients achieved remission defined by DORIS. Patients who met LLDAS or DORIS remission had significantly higher proportion of patients with high income and longer disease duration, compared with non-remission group. Moreover, the rates of anemia, creatinine elevation, increased erythrocyte sedimentation rate (ESR) and hypoalbuminemia was significantly lower in the LLDAS or DORIS group than in the non-remission group. Patients who received hydroxychloroquine for more than 12 months or immunosuppressant therapy for no less than 6 months earned higher rates of LLDAS and DORIS remission. The results of Logistic regression analysis showed that increased ESR, positive anti-dsDNA antibodies, low level of complement (C3 and C4), proteinuria, low household income were negatively related with LLDAS and DORIS remission. However, hydroxychloroquine usage for longer than 12 months were positively related with LLDAS and DORIS remission. CONCLUSION: LLDAS and DORIS remission of SLE patients remain to be improved. Treatment-to-target strategy and standar-dized application of hydroxychloroquine and immunosuppressants in SLE are recommended.
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Hidroxicloroquina , Lúpus Eritematoso Sistêmico , Humanos , Hidroxicloroquina/uso terapêutico , Lúpus Eritematoso Sistêmico/tratamento farmacológico , Imunossupressores/uso terapêutico , Índice de Gravidade de DoençaRESUMO
While all-inorganic halide perovskites (iHPs) are promising photovoltaic materials, the associated water sensitivity of iHPs calls for stringent humidity control to reach satisfactory photovoltaic efficiencies. Herein, we report a moisture-insensitive perovskite formation route under ambient air for CsPbI2 Br-based iHPs via cesium cyclopropane acids (C3 ) as a compound introducer. With this approach, appreciably enhanced crystallization quality and moisture tolerance of CsPbI2 Br are attained. The improvements are attributed to the modified evaporation enthalpy of the volatile side product of DMA-acid initiated by Cs-acids. As such, the water-involving reaction is directed toward the DMA-acids, leaving the target CsPbI2 Br perovskites insensitive to ambient humidity. We highlight that by controlling the C3 concentration, the dependence of power conversion efficiency (PCE) in CsPbI2 Br devices on the humidity level during perovskite film formation becomes favorably weakened, with the PCEs remaining relatively high (>15 %) associated with improved device stability for RH levels changed from 25 % to 65 %. The champion solar cells yield an impressive PCE exceeding 17 %, showing small degradations (<10 %) for 2000â hours of shell storage and 300â hours of 85/85 (temperature/humidity) tests. The demonstrated C3 -based strategy provides an enabler for improving the long-sought moisture-stability of iHPs toward high photovoltaic device performance.
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Mosquito viruses cause unpredictable outbreaks of disease. Recently, several unassigned viruses isolated from mosquitoes, including the Omono River virus (OmRV), were identified as totivirus-like viruses, with features similar to those of the Totiviridae family. Most reported members of this family infect fungi or protozoans and lack an extracellular life cycle stage. Here, we identified a new strain of OmRV and determined high-resolution structures for this virus using single-particle cryo-electron microscopy. The structures feature an unexpected protrusion at the five-fold vertex of the capsid. Disassociation of the protrusion could result in several conformational changes in the major capsid. All these structures, together with some biological results, suggest the protrusions' associations with the extracellular transmission of OmRV.
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Microscopia Crioeletrônica/métodos , Vírus de RNA de Cadeia Dupla/ultraestrutura , Proteínas Estruturais Virais/ultraestrutura , Aedes/virologia , AnimaisRESUMO
Two dimensional Dion-Jacobson (2D DJ) perovskite has emerged as a potential photovoltaic material because of its unique optoelectronic characteristics. However, due to its low structural flexibility and high formation energy, extra assistance is needed during crystallization. Herein, we study the solvent effect on film formation and trap states of 2D DJ perovskite. It is found that the nucleation process of 2D DJ perovskite can be retarded by extra coordination, which is proved by in situ optical spectra. As a benefit, out-of-plane oriented crystallization and ordered phase distribution are realized. Finally, in 1,5-pentanediammonium (PeDA) based 2D DJ perovskite solar cells (PSCs), one of the highest reported open-circuit voltage (VOC) values of 1.25 V with state-of-the-art efficiency of 18.41% is obtained due to greatly shallowed trap states and suppressed nonradiative recombination. The device also exhibits excellent heat tolerance, which maintains 80% of its initial efficiency after being kept under 85 °C after 3000 h.
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Although the photovoltaic performance of perovskite solar cells (PSCs) has reached the commercial standards, the unsatisfactory stability limits their further application. Hydrophobic interface and encapsulation can block the damage of water and oxygen, while the instability induced by intrinsic residual strain remains inevitable. Here, the residual strain in a two-dimensional (2D) Ruddlesden-Popper (RP) perovskite film is investigated by X-ray diffraction and atomic force microscopy. It's found that the spacer cations contribute to the residual strain even though they are not in the inorganic cages. Benefited from strain relaxation, the film quality is improved, leading to suppressed recombination, promoted charge transport and enhanced efficiency. More significantly, the strain-released devices maintain 86 % of the initial efficiency after being kept in air with 85 % relative humidity (RH) for 1080â h, 82 % under maximum power point (MPP) tracking at 50 °C for 804â h and 86 % after continuous heating at 85 °C for 1080â h.
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Solution-processed organic photovoltaic (OPV) as a new energy device has attracted much attention due to its huge potential in future commercial manufacturing. However, so far, most of the studies on high-performance OPV have been treated with halogenated solvents. Halogenated solvents not only pollute the environment, but are also harmful to human health, which will negatively affect the large-scale production of OPV in the future. Therefore, it is urgent to develop low-toxic or non-toxic non-halogen solvent-processable OPV. Compared with conventional fullerene OPVs, non-fullerene OPVs exist with stronger absorption, better-matched energy levels and lower energy loss. Processing photoactive layers with non-fullerenes as the acceptor material has broad potential advantages in non-halogenated solvents. This review introduces the research progress of non-fullerene OPV treated by three different kinds of green solvents as the non-halogenated and aromatic solvent, the non-halogenated and non-aromatic solvent, alcohol and water. Furthermore, the effects of different optimization strategies on the photoelectric performance and stability of non-fullerene OPV are analyzed in detail. The current optimization strategy can increase the power conversion efficiency of non-fullerene OPV processed with non-halogen solvents up to 17.33%, which is close to the performance of processing with halogen-containing solvents. Finally, the commercial potential of non-halogen solvent processing OPVs is discussed. The green solvent processing of non-fullerene-based OPVs will become a key development direction for the future of the OPV industry.
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Although the hot-casting (HC) technique is prevalent in developing preferred crystal orientation of quasi-2D perovskite films, the difficulty of accurately controlling the thermal homogeneity of substrate is unfavorable for the reproducibility of device fabrication. Herein, a facile and effective non-preheating (NP) film-casting method is proposed to realize highly oriented quasi-2D perovskite films by replacing the butylammonium (BA+ ) spacer partially with methylammonium (MA+ ) cation as (BA)2- x (MA)3+ x Pb4 I13 (x = 0, 0.2, 0.4, and 0.6). At the optimal x-value of 0.4, the resultant quasi-2D perovskite film possesses highly orientated crystals, associated with a dense morphology and uniform grain-size distribution. Consequently, the (BA)1.6 (MA)3.4 Pb4 I13 -based solar cells yield champion efficiencies of 15.44% with NP processing and 16.29% with HC processing, respectively. As expected, the HC-processed device shows a poor performance reproducibility compared with that of the NP film-casting method. Moreover, the unsealed device (x = 0.4) displays a better moisture stability with respect to the x = 0 stored in a 65% ± 5% relative humility chamber.
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All-inorganic perovskite solar cells (PSCs) are attracting considerable attention due to their promising thermal stability, but their inferior power-conversion efficiencies (PCE) hinder their realistic application. Here, we propose an approach through surface modification based on methyl ammonium halide (MAX) for inorganic CsPbI2Br solar cells processed at a low temperature. The combined benefits of the introduced MAX modifier enable the boosting of the power conversion efficiency to 14.8% with an impressive FF of 82.2% in CsPbI2Br PSCs. Our experimental analyses coupled with optical modeling indicate that the incorporated MAX leads to an effective passivation of the surface traps originating from Pb2+ and I- ions in CsPbI2Br and simultaneously mediates the crystallization of CsPbI2Br with slightly enlarged grains and reduced numbers of structural defects and pinhole. As a result, the interfacial trap-assisted recombination is suppressed and the charge extraction is promoted. Mechanistically, we show that in the presence of MAX, the deep-level traps in the perovskites are passivated, leaving the energy of the trapping centers to become shallower. In this situation, the negative impacts of the traps on carrier transport and recombination are mitigated.
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A comprehensive study unveiling the impact of heterovalent doping with Bi3+ on the structural, semiconductive, and photoluminescent properties of a single crystal of lead halide perovskites (CH3 NH3 PbBr3 ) is presented. As indicated by single-crystal XRD, a perfect cubic structure in Bi3+ -doped CH3 NH3 PbBr3 crystals is maintained in association with a slight lattice contraction. Time-resolved and power-dependent photoluminescence (PL) spectroscopy illustrates a progressively quenched PL of visible emission, alongside the appearance of a new PL signal in the near-infrared (NIR) regime, which is likely to be due to energy transfer to the Bi sites. These optical characteristics indicate the role of Bi3+ dopants as nonradiative recombination centers, which explains the observed transition from bimolecular recombination in pristine CH3 NH3 PbBr3 to a dominant trap-assisted monomolecular recombination with Bi3+ doping. Electrically, it is found that the mobility in pristine perovskite crystals can be boosted with a low Bi3+ concentration, which may be related to a trap-filling mechanism. Aided by temperature (T)-dependent measurements, two temperature regimes are observed in association with different activation energies (Ea ) for electrical conductivity. The reduction of Ea at lower T may be ascribed to suppression of ionic conduction induced by doping. The modified electrical properties and NIR emission with the control of Bi3+ concentration shed light on the opportunity to apply heterovalent doping of perovskite single crystals for NIR optoelectronic applications.
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Reaching the full potential of solar cells based on photo-absorbers of organic-inorganic hybrid perovskites requires highly efficient charge extraction at the interface between perovskite and charge transporting layer. This demand is generally challenged by the presence of under-coordinated metal or halogen ions, causing surface charge trapping and resultant recombination losses. These problems can be tackled by introducing a small molecule interfacial anchor layer based on dimethylbiguanide (DMBG). Benefitting from interactions between the nitrogen-containing functional groups in DMBG and unsaturated ions in CH3 NH3 PbI3 perovskites, the electron extraction of TiO2 is dramatically improved in association with reduced Schottky-Read-Hall recombination, as revealed by photoluminescence spectroscopy. As a consequence, the power conversion efficiency of CH3 NH3 PbI3 solar cells is boosted from 17.14 to 19.1 %, showing appreciably reduced hysteresis. The demonstrated molecular strategy based on DMBG enables one to achieve meliorations on key figures of merit in halide perovskite solar cells with improved stability.
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Here based on integral microcrystal (IMC) thin films of halide perovskites containing formamidinium (FA)/methylammonium (MA) mixed cations, afforded by a facile approach combining an anti-solvent and inverse temperature crystallization, we investigate the impact of the addition of MAPbBr3 on the phase, thermal and environmental stabilities as well as the opto-electronic properties in FA-based IMC films. By single-crystal XRD, FA based IMCs have been found to possess a perfect cubic structure showing a slight lattice contraction compared to pristine FAPbI3 crystals. In conjunction with optical and electrical analyses, the essential role of the introduced MA and Br ions in stabilizing the black phase in FA-based IMCs has been clarified, which explains the observed enhancement of photoluminescence and reduced trap densities. We also achieve stable pure FAPbI3 crystals that do not exhibit a yellow-phase transition after one month in air. By utilizing (FAPbI3)1-x(MAPbBr3)x IMCs as the photo-absorber, we realize highly photo-responsive photodiodes with a satisfactory stability in air and thermal stability upon heating. Of interest, the best photoresponsivity exceeding 300 A W-1 is achieved upon appropriate air-exposure, which is among the highest values reported for FA-based perovskite photodetectors. The air-modified optoelectronic behaviour can be related to the trap passivation through the surface physisorption of the environmental O2, leading to reduced trap densities and resultant harmful SRH recombination.
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The high genetic variability of RNA viruses is a significant factor limiting the discovery of effective biomarkers, the development of vaccines, and characterizations of the immune response during infection. Protein microarrays have been shown to be a powerful method in biomarker discovery and the identification of novel protein-protein interaction networks, suggesting that this technique could also be very useful in studies of infectious RNA viruses. However, to date, the amount of genetic material required to produce protein arrays, as well as the time- and labor-intensive procedures typically needed, have limited their more widespread application. Here, we introduce a method, protein microarray fabrication through gene synthesis (PAGES), for the rapid and efficient construction of protein microarrays particularly for RNA viruses. Using dengue virus as an example, we first identify consensus sequences from 3,604 different strains and then fabricate complete proteomic microarrays that are unique for each consensus sequence. To demonstrate their applicability, we show that these microarrays can differentiate sera from patients infected by dengue virus, related pathogens, or from uninfected patients. We anticipate that the microarray and expression library constructed in this study will find immediate use in further studies of dengue virus and that, more generally, PAGES will become a widely applied method in the clinical characterization of RNA viruses.
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Vírus da Dengue/metabolismo , Dengue/virologia , Análise Serial de Proteínas/métodos , Proteínas Virais/análise , Proteínas Virais/sangue , Adulto , Idoso , Dengue/sangue , Vírus da Dengue/genética , Feminino , Biblioteca Gênica , Variação Genética , Humanos , Masculino , Pessoa de Meia-Idade , Filogenia , Mapas de Interação de Proteínas , Proteômica/métodos , Proteínas Virais/genética , Adulto JovemRESUMO
Attaining control on charge injection properties is significant for meaningful applications of organic field-effect transistors (OFETs). Here, molecular electron-doping is applied with an air-stable dimer dopant for n-type OFETs based on (naphthalene diimide-diketopyrrolopyrrole) polymer hosts. Through investigating the doping effect on contact and transport properties, it is found that the electron transport increases in n-doped OFETs at low doping regime with remaining large on/off ratios. These favorable meliorations are reconciled by the mitigated impacts of contact resistance and interfacial traps, as well as the surface morphology exhibiting features of increased ordering. The occurrence of doping in the presence of dimer dopants is evidenced by the observed shift of Fermi level toward vacuum level coupled with compositional analysis. Without applying vacuum-deposition-based contact doping, charge injection efficiencies are gained without losing OFET characteristics using the solution-based methodology.
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Transporte de Elétrons , Compostos Orgânicos/química , Polímeros/química , Imidas/química , Cetonas/química , Naftalenos/química , Pirróis/química , Semicondutores , Transistores EletrônicosRESUMO
Energetic disorder and activation energy are important parameters that influence the charge carrier mobility in organic semiconductors. Herein, we investigate temperature-dependent ambipolar charge transport alongside its thermal activation energy in organic field-effect transistors (OFETs) based on a diketopyrrolopyrrole (DPP) based small molecule BTDPP2. The determined energetic disorder in BTDPP2 is analogous to those of highly crystalline molecules, such as pentacene, while lower than those of widely used fullerene derivatives (PCBM) or semi-crystalline polymers, such as P3HT. We demonstrate that the energetic disorder and activation energy in BTDPP2 are both impacted by the crystallinity, which is tuned by thermal annealing; moreover, to a certain extent, these two parameters can reduce with increasing the structural order. Moreover, the energetic disorder tends to decrease when BTDPP2 is subjected to thermal annealing. Through comparing the electron transport in BTDPP2 based OFETs and vertical diodes, in which the electron densities differentiate substantially, the different activation energies are roughly described in terms of achievable carrier densities in these two devices. To the best of our knowledge, this aspect has not been addressed on the electron transport in molecular semi-conductive materials. Our results shine light on fundamental understandings of charge transport properties in solution processed small molecules holding promise for opto-electronic applications.
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The hysteresis effect and instability are important concerns in hybrid perovskite photovoltaic devices that hold great promise in energy conversion applications. In this study, we show that the power conversion efficiency (PCE), hysteresis, and device lifetime can be simultaneously improved for methylammoniumlead halide (CH3 NH3 PbI3-x Clx ) solar cells after incorporating poly(methyl methacrylate) (PMMA) into the PC61 BM electron extraction layer (EEL). By choosing appropriate molecular weights of PMMA, we obtain a 30 % enhancement of PCE along with effectively lowered hysteresis and device degradation, adopting inverted planar device structure. Through the combinatorial study using Kelvin probe force microscopy, diode mobility measurements, and irradiation-dependent solar cell characterization, we attribute the enhanced device parameters (fill factor and open circuit voltage) to the surface passivation of CH3 NH3 PbI3-x Clx , leading to mitigating charge trapping at the cathode interface and resultant Shockley-Read-Hall charge recombination. Beneficially, modified by inert PMMA, CH3 NH3 PbI3-x Clx solar cells display a pronounced retardation in performance degradation, resulting from improved film quality in the PC61 BM layer incorporating PMMA which increases the protection for underneath perovskite films. This work enables a versatile and effective interface approach to deal with essential concerns for solution-processed perovskite solar cells by air-stable and widely accessible materials.
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INTRODUCTION: Entecavir, a nucleoside analog (NA), is effective for treatment of chronic hepatitis B virus (HBV) infection. METHODS: We report the case of a patient we encountered with entecavir-associated myopathy. We also performed a literature review of myopathies associated with nucleoside analogs. RESULTS: A 44-year-old man presented with a 3-month history of myalgia and progressive weakness. He had HBV infection and had received entecavir antiviral treatment for 5 years. Laboratory tests showed that serum creatine kinase levels were significantly elevated. Muscle histopathology showed abundant T-lymphocyte infiltration of muscle fibers, and HBV surface antigen and HBV core antigen were not present in muscle fibers. Entecavir-associated myopathy was subsequently diagnosed. The patient's symptoms eventually resolved, and serum CK levels decreased rapidly after he stopped receiving entecavir treatments. CONCLUSIONS: Patients who receive NA therapy should be closely monitored for myopathic side effects. Muscle Nerve 49:610-614, 2014.
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Antivirais/efeitos adversos , Guanina/análogos & derivados , Doenças Musculares/induzido quimicamente , Doenças Musculares/diagnóstico , Adulto , Guanina/efeitos adversos , Humanos , Masculino , Debilidade Muscular/induzido quimicamente , Debilidade Muscular/diagnósticoRESUMO
A mechanistic study of the DNA interfacial layer that enhances the photoresponse in n-type field-effect transistors (FET) and lateral photoconductors using a solution-processed fullerene derivative embedded with disperse-red dye, namely PCBDR, is reported. Incorporation of the thin DNA layer simultaneously leads to increasing the electron injection from non-Ohmic contacts into the PCBDR active layer in dark and to increasing the photocurrent under irradiation. Such features lead to the observation of the enhancement of the photoresponsivity in PCBDR FETs up to 10(3) . Kelvin probe microscopy displays that in the presence of the DNA layer, the surface potential of PCBDR has a greater change in response to irradiation, which is rationalized by a larger number of photoinduced surface carriers. Transient absorption spectroscopy confirms that the increase in photoinduced carriers in PCBDR under irradiation is primarily ascribed to the increase in exciton dissociation rates through the PCBDR/DNA interface and this process can be assisted by the interfacial dipole interaction.