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Photodetectors displaying an ultraviolet (UV) spectral response window are typically based on wide-bandgap semiconductors that have long been dominated by inorganic materials that suffer from bottlenecks of low flexibility and a limited material family. Here, we synthesized a novel organic small molecule and controlled its crystallization to suppress leakage currents and facilitate separation of the carriers, and the relationship between the nanoscale phase separation morphology and the optoelectrical performance of the photodetectors is disclosed. Our optimized organic photodetector (OPD) presents a UV spectral response window, with superior self-powered responsivities of 45 mA/W (under 250 nm light) and 70 mA/W (under 300 nm light), outperforming the Si photodiode and rivaling other reported UV self-powered photodetectors. Finally, an imaging system was constructed to demonstrate the application potential of the OPD in UV flexible imaging with high-resolution arrays of 400 pixels × 400 pixels (5 µm × 5 µm per pixel), which could work in bent states and successfully output images of micrometer-sized objects.
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RATIONALE: The development of appropriate analytical screening techniques for pharmaceuticals and personal care products (PPCPs) is the basis for studying the distribution and environmental impact of emerging contaminants (ECs). Mass spectrometry-based screening methods vary with the complexity of the target compounds. It is challenging to balance both positive and negative ion quantification with a low detection limit. To establish a set of experimental methods including extraction, chromatography-separation and mass spectrometry screening is one of the most important topics in PPCP research. This paper describes a universal and efficient qualification and quantification protocol for the simultaneous detection of 34 PPCPs in different environmental samples in a single analytical data acquisition run. METHODS: Thirty-four representative PPCPs, which are widely distributed in the environment with high ecological toxicity and complex chemical structures, were selected as representative target ECs. The extraction of the target PPCPs was achieved using only one solid-phase extraction cartridge without the need to adjust the pH of samples. The enriched samples were detected by LC-MS/MS in both positive and negative ion modes simultaneously. The protocol was evaluated based on the accuracy, precision, detection limits and matrix effects. RESULTS: This method achieved simultaneous detection of PPCPs in both positive and negative ion modes, with a single analytical cycle of 12 min. The observed SPE recoveries were between 40% and 115%. The instrumental detection limits (IDL) varied from 0.01 to 1 pg, and the method detection limits (MDL) were between 0.002 and 3.323 ng/l in different matrices. Most of the PPCPs were subjected to matrix suppression below 30%. The method was successfully applied for quantitative analysis of the PPCPs in different environmental samples, including river samples, wastewater treatment plant (WWTP) samples and soil samples. CONCLUSIONS: This protocol developed a rapid and efficient detection method to simultaneous qualitative and quantitative 34 representative PPCPs in the environment. The IDL ranged from 0.01 to 1 pg and the MDL ranged from 0.002 to 3.323 ng/l in different matrices. The detection limit was one order of magnitude lower compared to previous studies. The protocol also provided a wide application range for different environmental matrices, which permitted the migration and transformation of PPCPs to be explored.
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Cosméticos , Contaminantes Químicos del Agua , Cromatografía Liquida/métodos , Espectrometría de Masas en Tándem/métodos , Contaminantes Químicos del Agua/análisis , Cosméticos/análisis , Extracción en Fase Sólida/métodos , Preparaciones Farmacéuticas , Monitoreo del Ambiente/métodosRESUMEN
Sauce-flavor Baijiu is one of the most complex and typical types of traditional Chinese liquor, whose trace components have an important impact on its taste and quality. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) is one of the most favorable analytical tools to reveal trace molecular components in complex samples. This study analyzed the chemical diversity of several representative sauce-flavor Baijiu using the combination of electrospray ionization (ESI) and FT-ICR MS. The results showed that ESI+ and ESI- exhibited different chemical features characteristic of trace components. Overall, sauce-flavor Baijiu was dominated by CHO class compounds, and the main specific compound types were aliphatic, highly unsaturated with low oxygen, and peptide-like compounds. The mass spectral parameters resolved by FT-ICR MS of several well-known brands were relatively similar, whereas the greatest variability was observed from an internally supplied brand. This study provides a new perspective on the mass spectrometry characteristics of trace components of sauce-flavor Baijiu and offers a theoretical foundation for further optimization of the gradients in Baijiu.
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RATIONALE: Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) combined with different ionization techniques provides a powerful means to characterize dissolved organic matter (DOM) at the molecular level. Solid-phase extraction (SPE) is currently the most widely utilized method for extracting the DOM, but one-step elution using methanol does not provide a comprehensive picture of DOM. The development of efficient extraction and enrichment methods as well as characterization techniques from water samples remains a priority for DOM research, which is investigated in this study. METHODS: The DOM was extracted from lake water by SPE using one-step elution (methanol or dichloromethane) and multistep elution (water, methanol, acetone, and dichloromethane). A combination of electrospray ionization (ESI), atmospheric pressure photoionization (APPI), and matrix-free laser desorption ionization (LDI) was utilized for FT-ICR MS analysis in both positive (+) and negative (-) ion modes. RESULTS: The total recovery of the multistep elution was 23.5% higher as compared to the investigated one-step elution procedure (85% vs. 61.6%); however, a comparison of the observed molecular species and the range of diversity under different ionization techniques along with the statistical analyses showed that proper selection of solvent and ionization method was required to explore specific compounds from the sample. CONCLUSIONS: For DOM species containing different heteroatoms, a combination of ESI, APPI, and LDI can offer a comprehensive profile of DOM in aquatic ecosystems. The specific molecular formulae of each ionization technique are characterized as follows: ESI- mode exhibited strong selectivity for lignin-like and tannins-like species with high oxygen content, as well as organosulfates. ESI+ favored lipid species and peptide/protein compounds. Unsaturated and condensed aromatic hydrocarbons with low oxygen were preferably ionized by both APPI and LDI.
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Ciclotrones , Materia Orgánica Disuelta , Presión Atmosférica , Ecosistema , Análisis de Fourier , Rayos Láser , Espectrometría de Masas/métodos , Metanol , Cloruro de Metileno , Oxígeno , Extracción en Fase Sólida/métodos , Espectrometría de Masa por Ionización de Electrospray/métodos , AguaRESUMEN
Long non-coding RNAs (lncRNAs) and circular RNAs (circRNAs) play vital roles in the tumorigenesis of esophageal squamous cell carcinoma (ESCC). Nevertheless, the mechanism and regulatory network associated with this process remain largely unknown. In this study, we performed a comprehensive analysis of the expression of mRNAs, lncRNAs, and circRNAs by RNA-seq. A total of 3265 mRNAs, 1084 lncRNAs, and 38 circRNAs were found to be differentially expressed. Among these, 269 mRNAs were found to encode transcription factors (TFs). Functional enrichment analysis indicated that the dysregulated TFs are associated with the Hedgehog, Jak-STAT, TGF-beta, and MAPK signaling pathways. Furthermore, we constructed co-expression networks to screen the core lncRNAs and circRNAs involved in the regulation of transcription factors in these four pathways. Finally, we constructed a competing endogenous RNA (ceRNA) network of ESCC based on the abovementioned pathways. Our findings provide important insight into the role of lncRNAs and circRNAs in ESCC; the differentially expressed lncRNAs and circRNAs may represent potential targets for ESCC diagnosis and therapy.
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Carcinoma de Células Escamosas/genética , Neoplasias Esofágicas/genética , Redes Reguladoras de Genes , ARN Circular/genética , ARN Largo no Codificante/genética , Carcinoma de Células Escamosas/metabolismo , Neoplasias Esofágicas/metabolismo , Regulación Neoplásica de la Expresión Génica , Proteínas Hedgehog/genética , Proteínas Hedgehog/metabolismo , Humanos , Sistema de Señalización de MAP Quinasas , ARN Circular/metabolismo , ARN Largo no Codificante/metabolismo , Factores de Transcripción STAT/genética , Factores de Transcripción STAT/metabolismo , Factor de Crecimiento Transformador beta/genética , Factor de Crecimiento Transformador beta/metabolismoRESUMEN
Lignin is the second most abundant natural biopolymer, which is a potential alternative to conventional fossil fuels. It is also a promising material for the recovery of valuable chemicals such as aromatic compounds as well as an important biomarker for terrestrial organic matter. Lignin is currently produced in large quantities as a by-product of chemical pulping and cellulosic ethanol processes. Consequently, analytical methods are required to assess the content of valuable chemicals contained in these complex lignin wastes. This review is devoted to the application of mass spectrometry, including data analysis strategies, for the elemental and structural elucidation of lignin products. We describe and critically evaluate how these methods have contributed to progress and trends in the utilization of lignin in chemical synthesis, materials, energy, and geochemistry.
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Lignina/química , Espectrometría de MasasRESUMEN
Non-fullerene all-small-molecule organic solar cells (NFSM-OSCs) have shown potential as OSCs, owing to their high purity, easy synthesis and good reproducibility. However, challenges in the modulation of phase separation morphology have limited their development. Herein, two novel small molecular donors, BTEC-1F and BTEC-2F, derived from the small molecule DCAO3TBDTT, are synthesized. Using Y6 as the acceptor, devices based on non-fluorinated DCAO3TBDTT showed an open circuit voltage (Voc ) of 0.804â V and a power conversion efficiency (PCE) of 10.64 %. Mono-fluorinated BTEC-1F showed an increased Voc of 0.870â V and a PCE of 11.33 %. The fill factor (FF) of di-fluorinated BTEC-2F-based NFSM-OSC was improved to 72.35 % resulting in a PCE of 13.34 %, which is higher than that of BTEC-1F (61.35 %) and DCAO3TBDTT (60.95 %). To our knowledge, this is the highest PCE for NFSM-OSCs. BTEC-2F had a more compact molecular stacking and a lower crystallinity which enhanced phase separation and carrier transport.
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BACKGROUND: Anastomotic leak after esophagectomy is one of the most challenging complications resulting in a high morbidity and mortality and prolonged hospitalization. The aim of this retrospective study was to access the impact of endoscopy intervention in anastomotic leak. METHODS: A retrospective review was conducted at our hospital from January 2008 to December 2016. In total, 263 patients who were diagnosed with an anastomotic leak after esophagectomy and underwent endoscopy examination were included in this study. First, all patients were divided into two groups based on a single criteria-whether they received endoscopy intervention or not-and comparisons were conducted between the two groups. Second, we categorized all patients into three groups based on the diameter of the anastomotic leak (group I: <5 mm; group II: 5-15 mm; group III: >15 mm). Detailed analyses were made for each group. Factors we considered included demographic factors, the length of postoperative hospital stay, the amount of medical expenditure, limited days of oral intake, and the incurrence of complications. Data relating to those factors were collected and then analyzed using standard statistic tools. RESULTS: In general, the difference between endoscopy intervention and conservative measure was significant. Moreover, the hospital stay (p < 0.001; p = 0.018), medical expenditure (p < 0.001; p = 0.003), limited days of oral intake (p < 0.001; p = 0.019), and postoperative complications such as hemorrhage (p < 0.001; p = 0.036), tracheoesophageal fistula (p = 0.002; p = 0.017), and anastomosis stricture (p = 0.03; p = 0.026) were significantly lower among patients who received endoscopy intervention in groups II and III. However, no significant difference was identified between endoscopy intervention and conservative measure in group I. CONCLUSIONS: Endoscopy intervention is safe and effective in the diagnosis and treatment of postesophagectomy anastomotic leak. Especially for patients with a diameter of anastomotic leaks greater than 5 mm, the advantages of endoscopy intervention should not be neglected.
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Fuga Anastomótica/terapia , Coagulación con Plasma de Argón , Tratamiento Conservador , Esofagectomía/efectos adversos , Gastroscopía , Anciano , Anciano de 80 o más Años , Fuga Anastomótica/diagnóstico , Fuga Anastomótica/etiología , Coagulación con Plasma de Argón/efectos adversos , Tratamiento Conservador/efectos adversos , Femenino , Gastroscopía/efectos adversos , Gastroscopía/instrumentación , Humanos , Tiempo de Internación , Masculino , Persona de Mediana Edad , Recuperación de la Función , Estudios Retrospectivos , Factores de Riesgo , Stents Metálicos Autoexpandibles , Factores de Tiempo , Resultado del TratamientoRESUMEN
The current paper aims to study the effect of adenovirus-mediated IL-24 (Ad-IL-24) on human lung adenocarcinoma in vitro and in vivo and determine its possible mechanism of action. The growth-suppressing and apoptosis-inducing effects of Ad-IL-24, radiotherapy, and Ad-IL-24+ radiotherapy (hereinafter referred to as the joint group) on SPC-A1 lung carcinoma cells were assessed by using 3-(4,5-dimethyliazolyl-2)-2,5-diphnyltetrazolium bromide and flow cytometry. A human lung model was established with SPC-A1 cells in nude mice. Groups of mice were subjected to multi-point injections to their tumors. Gross tumor volumes were measured dynamically. The ratios of tumor suppression and radiosensitization effect were evaluated according to the method of probability sum Q values. The expressions of Bax, Bcl-2, Survivin, and Caspase-3 in tumor samples were detected by immunohistochemistry. The ratios of inhibition and apoptosis in the joint group were higher than those in the individual Ad-IL-24 and radiotherapy groups. In vitro, the joint group suppressed tumor growth conspicuously, showing a weight inhibition rate of about 64 %. The expressions of FasL, Bax and Caspase-3 were upregulated in the joint group, while the expressions of Cox,Bcl-2,VEGF,CD34 and Survivin were downregulated. The current study proves that Ad-IL-24 suppresses growth of SPC-A1 cells both in vitro and in vivo. Its functions appear to be related to cell apoptosis and antiangiogenesis.
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Adenocarcinoma/terapia , Interleucinas/genética , Neoplasias Pulmonares/terapia , Tolerancia a Radiación/genética , Ensayos Antitumor por Modelo de Xenoinjerto , Adenocarcinoma/genética , Adenocarcinoma/patología , Adenoviridae/genética , Animales , Apoptosis/genética , Apoptosis/efectos de la radiación , Western Blotting , Línea Celular Tumoral , Supervivencia Celular/genética , Supervivencia Celular/efectos de la radiación , Terapia Combinada , Relación Dosis-Respuesta en la Radiación , Citometría de Flujo , Terapia Genética/métodos , Células HEK293 , Humanos , Interleucinas/metabolismo , Neoplasias Pulmonares/genética , Neoplasias Pulmonares/patología , Masculino , Ratones Endogámicos BALB C , Ratones Desnudos , Radioterapia/métodos , Reacción en Cadena de la Polimerasa de Transcriptasa Inversa , Carga Tumoral/genética , Carga Tumoral/efectos de la radiaciónRESUMEN
Stretchable organic photovoltaics (OPVs) have attracted significant attention as promising power sources for wearable electronic systems owing to their superior robustness under repetitive tensile strains and their good compatibility. However, reconciling a high power-conversion efficiency and a reasonable flexibility is a tremendous challenge. In addition, the development of stretchable OPVs must be accelerated to satisfy the increasing requirements of niche markets for mechanical robustness. Stretchable OPV devices can be classified as either structurally or intrinsically stretchable. This work reviews recent advances in stretchable OPVs, including the design of mechanically robust transparent electrodes, photovoltaic materials, and devices. Initially, an overview of the characteristics and recent research progress in the areas of structurally and intrinsically stretchable OPVs is provided. Subsequently, research into flexible and stretchable transparent electrodes that directly affect the performances of stretchable OPVs is summarized and analyzed. Overall, this review aims to provide an in-depth understanding of the intrinsic properties of highly efficient and deformable active materials, while also emphasizing advanced strategies for simultaneously improving the photovoltaic performance and mechanical flexibility of the active layer, including material design, multi-component settings, and structural optimization.
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Organic solar cells (OSCs) with high performance were prepared using poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and [2-(3,6-dibromo-9H-carbazol-9-yl)ethyl]phosphonic acid (Br-2PACz) double-layer films as the anode interface. By spin-coating a layer of Br-2PACz on PEDOT:PSS to form a PEDOT:PSS/Br-2PACz dual-anode interface, both the Jsc and FF of the device can be increased simultaneously, resulting in a high Jsc of 27.84 mA cm-2 and a high FF of 78.18%. The promising result indicates that the PEDOT:PSS/Br-2PACz dual-anode interface is an effective way to improve the performance of OSCs. The improvement of device performance is mainly attributed to (1) improved interface conductivity; (2) increased hole mobility and more balanced carrier transport efficiency; and (3) optimized morphology, which well explains the increase of Jsc and FF of the device. In addition, the OSC based on the PEDOT:PSS/Br-2PACz dual-anode interface exhibits exceptional stability, as it can maintain 94.7% of its initial efficiency even after 500 h of storage in a nitrogen environment. This work provides a promising strategy for improving the efficiency and stability of OSCs by dual-anode interface modulation.
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Pharmaceuticals and personal care products (PPCPs) are emerging contaminants that have raised urgent environmental issues. The dissolved organic matter (DOM) plays a pivotal role on PPCPs' migration and transformation. To obtain a comprehensive understanding of the occurrence and distribution of PPCPs, a seasonal sampling focused on the riverine system in coastal zone, Tianjin, Bohai Rim was conducted. The distribution and transformation of thirty-three PPCPs and their interaction with DOM were investigated, and their sources and ecological risks were further evaluated. The total concentration of PPCPs ranges from 0.01 to 197.20 µg/L, and such value is affected by regional temperature, DOM and land use types. PPCPs migration at soil-water interface is controlled by temperature, sunlight, water flow and DOM. PPCPs have a high affinity to the protein-like DOM, while the humus-like DOM plays a negative influence and facilitates PPCPs' degradation. It is also found that protein-like DOM can represent point source pollution, while humus-like substances indicate non-point source (NPS) emission. Specific PPCPs can be used as markers to trace the source of domestic discharge. Additionally, daily use PPCPs such as ketoprofen, caffeine and iopromide are estimated to be the main risk substances, and their ecological risk varies on space, season and river hydraulic condition.
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Cosméticos , Contaminantes Químicos del Agua , Estaciones del Año , Materia Orgánica Disuelta , Monitoreo del Ambiente , Contaminantes Químicos del Agua/análisis , Cosméticos/análisis , China , Agua , Suelo , Ríos , Preparaciones FarmacéuticasRESUMEN
Organic solar cells, as a cutting-edge sustainable renewable energy technology, possess a myriad of potential applications, while the bottleneck problem of less than 20% efficiency limits the further development. Simultaneously achieving an ordered molecular arrangement, appropriate crystalline domain size, and reduced nonradiative recombination poses a significant challenge and is pivotal for overcoming efficiency limitations. This study employs a dual strategy involving the development of a novel acceptor and ternary blending to address this challenge. A novel non-fullerene acceptor, SMA, characterized by a highly ordered arrangement and high lowest unoccupied molecular orbital energy level, is synthesized. By incorporating SMA as a guest acceptor in the PM6:BTP-eC9 system, it is observed that SMA staggered the liquid-solid transition of donor and acceptor, facilitating acceptor crystallization and ordering while maintaining a suitable domain size. Furthermore, SMA optimized the vertical morphology and reduced bimolecular recombination. As a result, the ternary device achieved a champion efficiency of 20.22%, accompanied by increased voltage, short-circuit current density, and fill factor. Notably, a stabilized efficiency of 18.42% is attained for flexible devices. This study underscores the significant potential of a synergistic approach integrating acceptor material innovation and ternary blending techniques for optimizing bulk heterojunction morphology and photovoltaic performance.
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The emerging Y-series nonfullerene acceptors (Y-NFA) has prompted the rapid progress of power conversion efficiency (PCE) of all-small-molecule organic solar cells (ASM-OSCs) from around 12% to 17%. The excellent PCE improvement benefits from not only the outstanding properties of Y-series acceptors but also the successful development of small-molecule donors. The short-circuit current density, fill factor, and nonradiative recombination are all optimized to the unprecedented values, providing a scenery that is obviously different from the ITIC-series based ASM-OSCs. In this review, OSCs utilizing small-molecule donors and Y-NFA are summarized and classified in order to provide an up-to-date development overview and give an insight on structure-property correlation. Then, the characteristics of bulk-heterojunction (BHJ) formation of ASM-OSCs are discussed and compared with that of polymer-based OSCs. Finally, the challenges and outlook on designing ground-breaking small-molecule donor and forming an ideal BHJ morphology are discussed.
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Natural dissolved organic matter (DOM) is one of the Earth's dynamic carbon pools and a key intermediate in the global carbon cycle. Photochemical processes potentially affect DOM composition and activity in surface water. Suspended particulate matter (SPM) is the integral component of slow-moving rivers, and holds the potential for photochemical reactivity. To further investigate the influence of SPM on DOM photochemical transformation, this study conducted experiments comparing samples with and without SPM irradiated under simulated sunlight. Surface water samples from slow-moving urban rivers were collected. DOM optical characteristics and molecular features obtained by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) were investigated. Photolabile DOM was enriched in unsaturated and highly aromatic terrestrial substances. Photoproduced DOM had low aromaticity and was dominated by saturated aliphatics, protein-like substances, and carbohydrates. Study results indicated that the presence of SPM had a nonnegligible impact on the molecular traits of DOM, such as composition, molecular diversity, photolability, and bioavailability during photochemical reactions. In the environment affected by SPM, molecules containing heteroatoms exhibit higher photosensitivity. SPM promotes the photochemical transformation of a wider range of chemical types of photolabile DOM, particularly nitrogen-containing compounds. This study provides an essential insight into the more precise simulation of photochemical reactions of DOM influenced by SPM occurring in natural rivers, contributing to our understanding of the global carbon cycle from new theoretical perspectives.
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There is always a dilemma between strong π-π stacking/crystallinity and suitable domain size for all-small-molecule organic solar cells (ASM-OSCs), which puts forward higher requirements for the design of molecular donors. In this work, a series of novel molecular donors with different positional 2-ethylhexy (EH) attachments are designed and synthesized, named SM-R, SM-REH, SM-EH-R, and SM-EH-REH. It is found that EH-substitution on end groups (SM-REH) enables improved π-π interaction and crystallinity but with decreased solubility and phase size, leading to the improved efficiency of 15.6% as compared to 14.0% of SM-R. In contrast, EH-substitution on the π-bridge (SM-EH-R) significantly suppresses π-π stacking and increases the solubility, resulting in the lower efficiency of 11.9%. The further EH-substitution on end-groups of SM-EH-R, namely, SM-EH-REH, recovers the π-π stacking strength and obtains a moderate efficiency of 14.4%. Despite the higher crystallinity and increased π-π stacking in some molecules, the blend films show the gradually decreased domain size in the sequence of SM-R, SM-REH, SM-EH-R, and SM-EH-REH owing to the steric hindrance of the EH-chain. Overall, this work indicates that obtaining the higher π-π stacking/crystallinity and decreased domain size is achievable by tuning the EH-chain substitution, which paves the way to further improve the photovoltaic performance of ASM-OSCs.
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High power conversion efficiency (PCE) and mechanical robustness are key requirements for wearable applications of organic solar cells (OSCs). However, almost all highly efficient photoactive films comprising polymer donors (PD ) and small molecule acceptors (SMAs) are mechanically brittle. In this study, highly efficient (PCE = 17.91%) and mechanically robust (crack-onset strain [COS] = 11.7%) flexible OSCs are fabricated by incorporating a ductile oligomeric acceptor (DOA) into the PD :SMA system, representing the most flexible OSCs to date. The photophysical, mechanical, and photovoltaic properties of D18:N3 with different DOAs are characterized. By introducing DOA DOY-C4 with a longer flexible alkyl linker and lower polymerization, the D18:N3:DOY-C4-based flexible OSCs exhibit a significantly higher PCE (17.91%) and 50% higher COS (11.7%) than the D18:N3-based device (PCE = 17.06%, COS = 7.8%). The flexible OSCs based on D18:N3:DOY-C4 retain 98% of the initial PCE after 2000 consecutive bending cycles, showing greater mechanical stability than the reference device (maintaining 89% of initial PCE). After careful investigation, it is hypothesized that the enhancement in mechanical properties is mainly due to the formation of tie chains or entanglement in the ternary blend films. These results demonstrate that DOAs have great potential for achieving high-performance flexible OSCs.
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Fine-tuning the phase-separated morphology is of great importance to achieve efficient all-small-molecule organic solar cells (ASM-OSCs). In this work, a pair of isomers are designed and synthesized, namely, BDT-UF and BDT-DF, in which the fluorine atom in BDT-UF is close to the alkyl chain of side-chain thiophene, while that in BDT-DF is close to the center core. Owing to the noncovalent interaction between fluorine and hydrogen, BDT-DF shows a smaller dihedral angle between the thiophene side chain and the BDT core, which causes better molecular planarity. When mixed with N3, BDT-UF shows better miscibility, higher crystallinity, and more ordered molecule stacking in the blend film. Finally, the device of BDT-DF:N3 gains a power conversion efficiency (PCE) of 14.5%, while that of BDT-UF:N3 shows an increase in Voc, Jsc, and FF and gains a PCE of 15.1%. Our work exhibits a way of adjusting the substitution site of fluorine atoms to improve the PCE of ASM-OSCs.
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The sources and composition of dissolved organic matter (DOM) in rivers are critical to water quality and aquatic ecosystems. Studies on detailed composition of organic matter in rivers in the farming-pastoral ecotone are relatively limited in the research community. To better understand the characteristics and dynamics of DOM, Yang River in North China was selected as the study area because of its profound influences on the farming-pastoral ecotone nearby. A combination of fluorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) techniques revealed that the DOM composition of Yang River is driven by land use. DOM in Yang River is predominantly imported from allochthonous inputs, together with agricultural runoff, pastureland, and urban sewage, causing a comprehensive impact on DOM. In detail, DOM associated with cropland inputs was dominated by lignin-like species, with higher nitrogen content. In comparison, DOM related to grassland is more diverse and susceptible to degradation. An increase in urban areas led to an increase in sulfur-containing compounds, while their oxygen, nitrogen, and aromaticity contents were significantly lower than those in cropland. Interestingly, urban-influenced lignin-like compounds may be associated with the effluents from the pulp and paper mill. Additionally, synthetic surfactants from the lower section of the river were also structurally identified by tandem mass spectrometry. Overall, this study could provide valuable insights into the DOM sources and their transformation dynamics at a molecular level, which could be an indicator for riverine water quality management and be applied to other farming-pastoral ecotones straightforward.
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Materia Orgánica Disuelta , Ríos , Agricultura , China , Ecosistema , Fluorescencia , Lignina , Nitrógeno , Ríos/química , Espectrometría de FluorescenciaRESUMEN
Asymmetric substitution of end-groups is first applied in molecular donors. Three commonly used end-groups of 2-ethylhexyl cyanoacetate (CA), 2-ethylhexyl rhodanine (Reh), and 1H-indene-1,3(2H)-dione (ID) are combined to construct a series of symmetric and asymmetric donors. Correspondingly, the asymmetric donors SM-CA-Reh and SM-CA-ID show largely increased dipole moments (2.14 and 3.39 D, respectively) and enhanced aggregation propensity, as compared to those of symmetric donors of SM-CA, SM-Reh, and SM-ID. Using N3 as acceptor, interestingly, SM-CA-Reh integrates the photovoltaic characteristics of high fill factor (FF) for SM-CA and high short-circuit current density for SM-Reh, and delivers a record power conversion efficiency (PCE) of 16.34% with a high FF of 77.5%, which is much higher than 15.41% for SM-CA and 14.76% for SM-Reh. However, SM-CA-ID and SM-ID give the lower PCE of 8.20% and 2.76%. Characterization results suggest that the π-π interaction mainly dictates the packing morphology of blend films instead of dipole effect or crystallinity. Mono-substitution of Reh facilitates the molecular demixing appropriately but keeps the characteristic of the fine bicontinuous network of SM-CA:N3. SM-CA-Reh:N3 shows more efficient exciton extraction, higher hole transport, and better miscibility. These results well explain the merits integration and improved photovoltaic performance.