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1.
Mater Horiz ; 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38567487

RESUMO

Recently, inverted perovskite solar cells (PeSCs) have witnessed significant advancements; however, their long-term stability remains a challenge because of the oxidation of silver cathodes to form AgI by mobile iodides. To overcome this problem, we propose the integration of an electron-deficient naphthalene diimide-based zwitterion (NDI-ZI) as the cathode interlayer. Compared to the physical ion-blocking layer, it effectively captures ions by forming ionic bonds via electrostatic Coulombic interaction to suppress the migration of iodide and Ag ions. The NDI-ZI interlayer also suppresses the shunt paths and modulates the work function of the Ag electrode by forming interface dipoles, thereby enhancing charge extraction. FA0.85Cs0.15PbI3 based PeSCs incorporating NDI-ZI exhibited a noticeably high power conversion efficiency of up to 23.3% and outstanding stability, maintaining ∼80% of their initial performance over 1500 h at 85 °C and over 500 h under continuous 1-sun illumination. This study highlights the potential of a zwitterionic cathode interlayer in diverse perovskite optoelectronic devices, leading to their improved efficiency and stability.

2.
Ann Am Thorac Soc ; 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38568439

RESUMO

RATIONALE: It is unknown whether air pollution is associated with radiographic features of interstitial lung disease in individuals with chronic obstructive pulmonary disease (COPD). OBJECTIVES: To determine whether air pollution increases prevalence of interstitial lung abnormalities (ILA) or percent high-attenuation area (HAA) on computed tomography (CT) in individuals with a heavy smoking history and COPD. METHODS: We performed a cross-sectional study of SPIROMICS (Subpopulations and Intermediate Outcome Measures in COPD Study), focused on current or former smokers with COPD. 10-year exposure to particulate matter < 2.5 µm (PM2.5), nitrogen oxides (NOx), nitrogen dioxide (NO2), and ozone (O3) prior to enrollment CTs (completed between 2010-2015) were estimated with validated spatiotemporal models at residential addresses. We applied adjusted multivariable modified Poisson regression and linear regression to investigate associations between pollution exposure and relative risk of ILA or increased percent HAA (between -600 and -250 Hounsfield units) respectively. We assessed for effect modification by MUC5B-promoter polymorphism (GT/TT vs GG at rs3705950), smoking status, sex, and percent emphysema. RESULTS: Among 1272 participants with COPD assessed for HAA, 424 were current smokers, 249 were carriers of the variant MUC5B allele (GT/TT). 519 participants were assessed for ILA. We found no association between pollution exposure and ILA or HAA. Associations between pollutant exposures and risk of ILA were modified by the presence of MUC5B polymorphism (p-value interaction term for NOx = 0.04 and PM2.5 = 0.05) and smoking status (p-value interaction term for NOx = 0.05, NO2 = 0.01, and O3 = 0.05). With higher exposure to NOx and PM2.5, MUC5B variant carriers had increased risk of ILA (Relative Risk [RR] per 26ppb NOx 2.41; 95% Confidence Interval [CI] 0.97 to 6.0) and RR per 4 µg·m-3 PM2.5 1.43; 95% CI 0.93 to 2.2). With higher exposure to NO2, former smokers had increased risk of ILA (RR per 10ppb 1.64; 95% CI 1.0 to 2.7). CONCLUSIONS: Exposure to ambient air pollution was not associated with interstitial features on CT in this population of heavy smokers with COPD. MUC5B modified the association between pollution and ILA, suggesting that gene-environment interactions may influence prevalence of interstitial lung features in COPD.

3.
Artigo em Inglês | MEDLINE | ID: mdl-38687147

RESUMO

Background: Omega-3 polyunsaturated fatty acids (PUFAs) have been associated with systemic anti-inflammatory responses. Dietary intake of omega-3 PUFAs eicosapentaenoic acid (EPA) and docosahexaenoic acid (DHA) has also been associated with lower COPD morbidity using self-report food frequency questionnaires. Objective: To investigate the relationship between measured PUFA intake using plasma EPA+DHA levels and COPD morbidity. Methods: Former smokers with moderate-severe COPD living in low-income communities were enrolled in a 6-month prospective cohort study. Participants completed standardized questionnaires, spirometry, and plasma samples at 3-month intervals. Total plasma PUFAs were analyzed using gas chromatography/ mass spectrometry for DHA and EPA concentrations. Linear or logistic mixed model regression was used to evaluate EPA+DHA's and COPD morbidity's association, accounting for demographics, lung function, pack years, comorbidities, and neighborhood poverty. Results: 133 plasma EPA+DHA samples from 57 participants were available. Participants exhibited average plasma EPA and DHA levels of 14.7±7.3 µg/mL and 40.2±17.2 µg/mL, respectively, across the three clinic visits. Each standard deviation increase in EPA+DHA levels was associated with 2.7 points lower SGRQ score (95% CI -5.2, -0.2) and lower odds of moderate exacerbation (OR 0.4; 95% CI 0.2, 0.9) but lacked significant association with CAT score (95% CI -2.4, 0.8), mMRC (95% CI -02, 0.2), or severe exacerbations (95% CI 0.3, 1.4). Conclusion: Plasma EPA+DHA levels are associated with better respiratory-specific quality of life and lower odds of moderate exacerbations in patients with moderate-to-severe COPD. Further research is warranted to investigate the efficacy of an omega-3 dietary intervention in the management of COPD morbidities.

4.
ACS Appl Mater Interfaces ; 16(10): 12886-12896, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38425182

RESUMO

Eco-friendly solution processing and the low-cost synthesis of photoactive materials are important requirements for the commercialization of organic solar cells (OSCs). Although varieties of aqueous-soluble acceptors have been developed, the availability of aqueous-processable polymer donors remains quite limited. In particular, the generally shallow highest occupied molecular orbital (HOMO) energy levels of existing polymer donors limit further increases in the power conversion efficiency (PCE). Here, we design and synthesize two water/alcohol-processable polymer donors, poly[(thiophene-2,5-diyl)-alt-(2-((13-(2,5,8,11-tetraoxadodecyl)-2,5,8,11-tetraoxatetradecan-14-yl)oxy)-6,7-difluoroquinoxaline-5,8-diyl)] (P(Qx8O-T)) and poly[(selenophene-2,5-diyl)-alt-(2-((13-(2,5,8,11-tetraoxadodecyl)-2,5,8,11-tetraoxatetradecan-14-yl)oxy)-6,7-difluoroquinoxaline-5,8-diyl)] (P(Qx8O-Se)) with oligo(ethylene glycol) (OEG) side chains, having deep HOMO energy levels (∼-5.4 eV). The synthesis of the polymers is achieved in a few synthetic and purification steps at reduced cost. The theoretical calculations uncover that the dielectric environmental variations are responsible for the observed band gap lowering in OEG-based polymers compared to their alkylated counterparts. Notably, the aqueous-processed all-polymer solar cells (aq-APSCs) based on P(Qx8O-T) and poly[(N,N'-bis(3-(2-(2-(2-methoxyethoxy)-ethoxy)ethoxy)-2-((2-(2-(2-methoxyethoxy)ethoxy)ethoxy)-methyl)propyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl)-alt-(2,5-thiophene)] (P(NDIDEG-T)) active layer exhibit a PCE of 2.27% and high open-circuit voltage (VOC) approaching 0.8 V, which are among the highest values for aq-APSCs reported to date. This study provides important clues for the design of low-cost, aqueous-processable polymer donors and the fabrication of aqueous-processable OSCs with high VOC.

5.
Artigo em Inglês | MEDLINE | ID: mdl-38507607

RESUMO

RATIONALE: Individuals with COPD have airflow obstruction and maldistribution of ventilation. For those living at high altitude, any gas exchange abnormality is compounded by reduced partial pressures of inspired oxygen. OBJECTIVES: Does residence at higher-altitude exposure affect COPD outcomes, including lung function, imaging characteristics, symptoms, health status, functional exercise capacity, exacerbations, or mortality? METHODS: From the SPIROMICS cohort, we identified individuals with COPD living below 1,000 ft (305 m) elevation (n= 1,367) versus above 4,000 ft (1,219 m) elevation (n= 288). Multivariable regression models were used to evaluate associations of exposure to high altitude with COPD-related outcomes. MEASUREMENTS AND MAIN RESULTS: Living at higher altitude was associated with reduced functional exercise capacity as defined by 6MWD (-32.3 m, (-55.7 to -28.6)). There were no differences in patient-reported outcomes as defined by symptoms (CAT, mMRC), or health status (SGRQ). Higher altitude was not associated with a different rate of FEV1 decline. Higher altitude was associated with lower odds of severe exacerbations (IRR 0.65, (0.46 to 0.90)). There were no differences in small airway disease, air trapping, or emphysema. In longitudinal analyses, higher altitude was associated with increased mortality (HR 1.25, (1.0 to 1.55)); however, this association was no longer significant when accounting for air pollution. CONCLUSIONS: Chronic altitude exposure is associated with reduced functional exercise capacity in individuals with COPD, but this did not translate into differences in symptoms or health status. Additionally, chronic high-altitude exposure did not affect progression of disease as defined by longitudinal changes in spirometry.

6.
Angew Chem Int Ed Engl ; 63(17): e202319627, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38443313

RESUMO

High-performing n-type polymers are crucial for the advance of organic electronics field, however strong electron-deficient building blocks with optimized physicochemical properties for constructing them are still limited. The imide-functionalized polycyclic aromatic hydrocarbons (PAHs) with extended π-conjugated framework, high electron deficiency and good solubility serve as promising candidates for developing high-performance n-type polymers. Among the PAHs, phenanthrene (PhA) features a well-delocalized aromatic π-system with multiple modifiable active sites . However, the PhA-based imides are seldom studied, mainly attributed to the synthetic challenge. Herein, we report two functionalized PhAs, CPOI and CPCNI, by simultaneously incorporating imide with carbonyl or dicyanomethylene onto PhA. Notably, the dicyanomethylene-modified CPCNI exhibits a well stabilized LUMO energy level (-3.84 eV), attributed to the synergetic inductive effect from imide and cyano groups. Subsequently, based on CPOI and CPCNI, two polymers PCPOI-Tz and PCPCNI-Tz were developed. Applied to organic thin-film transistors, owing to the strong electron-deficiency of CPCNI, polymer PCPCNI-Tz shows an improved electron mobility and largely decreased threshold voltage compared with PCPOI-Tz. This work affords two structurally novel electron-deficient building blocks and highlights the effectiveness of dual functionalization of PhAs with strong electron-withdrawing groups for devising n-type polymers.

7.
Small ; : e2401176, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38529741

RESUMO

Incorporating a third component into binary organic solar cells (b-OSCs) has provided a potential platform to boost power conversion efficiency (PCEs). However, gaining control over the non-equilibrium blend morphology via the molecular design of the perylene diimide (PDI)-based third component toward efficient ternary organic solar cells (t-OSCs) still remains challenging. Herein, two novel PDI derivatives are developed with tailored molecular planarity, namely ufBTz-2PDI and fBTz-2PDI, as the third component for t-OSCs. Notably, after performing a cyclization reaction, the twisted ufBTz-2PDI with an amorphous character transferred to the highly planar fBTz-2PDI followed by a semi-crystalline character. When incorporating the semi-crystalline fBTz-2PDI into the D18:L8-BO system, the resultant t-OSC achieved an impressive PCE of 18.56%, surpassing the 17.88% attained in b-OSCs. In comparison, the addition of amorphous ufBTz-2PDI into the binary system facilitates additional charge trap sites and results in a deteriorative PCE of 14.37%. Additionally, The third component fBTz-2PDI possesses a good generality in optimizing the PCEs of several b-OSCs systems are demonstrated. The results not only provided a novel A-DA'D-A motif for further designing efficient third component but also demonstrated the crucial role of modulated crystallinity of the PDI-based third component in optimizing PCEs of t-OSCs.

8.
Trends Biotechnol ; 2024 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-38402137

RESUMO

Laboratory automation with robot-assisted processes enhances synthetic biology, but its economic impact on projects is uncertain. We have proposed an experiment price index (EPI) for a quantitative comparison of factors in time, cost, and sample numbers, helping measure the efficiency of laboratory automation in synthetic biology and biomolecular engineering.

9.
Angew Chem Int Ed Engl ; 63(11): e202319658, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38265195

RESUMO

Developing low-cost and high-performance n-type polymer semiconductors is essential to accelerate the application of organic thermoelectrics (OTEs). To achieve this objective, it is critical to design strong electron-deficient building blocks with simple structure and easy synthesis, which are essential for the development of n-type polymer semiconductors. Herein, we synthesized two cyano-functionalized highly electron-deficient building blocks, namely 3,6-dibromopyrazine-2-carbonitrile (CNPz) and 3,6-Dibromopyrazine-2,5-dicarbonitrile (DCNPz), which feature simple structures and facile synthesis. CNPz and DCNPz can be obtained via only one-step reaction and three-step reactions from cheap raw materials, respectively. Based on CNPz and DCNPz, two acceptor-acceptor (A-A) polymers, P(DPP-CNPz) and P(DPP-DCNPz) are successfully developed, featuring deep-positioned lowest unoccupied molecular orbital (LUMO) energy levels, which are beneficial to n-type organic thin-film transistors (OTFTs) and OTEs performance. An optimal unipolar electron mobility of 0.85 and 1.85 cm2 V-1 s-1 is obtained for P(DPP-CNPz) and P(DPP-DCNPz), respectively. When doped with N-DMBI, P(DPP-CNPz) and P(DPP-DCNPz) show high n-type electrical conductivities/power factors of 25.3 S cm-1 /41.4 µW m-1 K-2 , and 33.9 S cm-1 /30.4 µW m-1 K-2 , respectively. Hence, the cyano-functionalized pyrazine CNPz and DCNPz represent a new class of structurally simple, low-cost and readily accessible electron-deficient building block for constructing n-type polymer semiconductors.

10.
Adv Mater ; 36(18): e2308750, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38289228

RESUMO

Semi-transparent organic solar cells (ST-OSCs) possess significant potential for applications in vehicles and buildings due to their distinctive visual transparency. Conventional device engineering strategies are typically used to optimize photon selection and utilization at the expense of power conversion efficiency (PCE); moreover, the fixed spectral utilization range always imposes an unsatisfactory upper limit to its light utilization efficiency (LUE). Herein, a novel solid additive named 1,3-diphenoxybenzene (DB) is employed to dual-regulate donor/acceptor molecular aggregation and crystallinity, which effectively broadens the spectral response of ST-OSCs in near-infrared region. Besides, more visible light is allowed to pass through the devices, which enables ST-OSCs to possess satisfactory photocurrent and high average visible transmittance (AVT) simultaneously. Consequently, the optimal ST-OSC based on PP2+DB/BTP-eC9+DB achieves a superior LUE of 4.77%, representing the highest value within AVT range of 40-50%, which also correlates with the formation of multi-scale phase-separated morphology. Such results indicate that the ST-OSCs can simultaneously meet the requirements for minimum commercial efficiency and plant photosynthesis when integrated with the roofs of agricultural greenhouses. This work emphasizes the significance of additives to tune the spectral response in ST-OSCs, and charts the way for organic photovoltaics in economically sustainable agricultural development.

11.
Nucleic Acids Res ; 52(1): 492-506, 2024 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-38015471

RESUMO

Bacterial small RNAs (sRNAs) function in post-transcriptional regulatory responses to environmental changes. However, the lack of eukaryotic RNA interference-like machinery in bacteria has limited the systematic engineering of RNA repression. Here, we report the development of clustered regularly interspaced short palindromic repeats (CRISPR)-guided dead CRIPSR-associated protein 13a (dCas13a) ribonucleoprotein that utilizes programmable CRISPR RNAs (crRNAs) to repress trans-acting and cis-acting sRNA as the target, altering regulatory mechanisms and stress-related phenotypes. In addition, we implemented a modular loop engineering of the crRNA to promote modular repression of the target gene with 92% knockdown efficiency and a single base-pair mismatch specificity. With the engineered crRNAs, we achieved targetable single-gene repression in the polycistronic operon. For metabolic application, 102 crRNAs were constructed in the biofoundry and used for screening novel knockdown sRNA targets to improve lycopene (colored antioxidant) production in Escherichia coli. The CRISPR-dCas13a system will assist as a valuable systematic tool for the discovery of novel sRNAs and the fine-tuning of bacterial RNA repression in both scientific and industrial applications.


Assuntos
Repetições Palindrômicas Curtas Agrupadas e Regularmente Espaçadas , Técnicas Genéticas , Pequeno RNA não Traduzido , Sistemas CRISPR-Cas/genética , Escherichia coli/genética , Escherichia coli/metabolismo , RNA Bacteriano/genética , RNA Bacteriano/metabolismo , RNA Mensageiro/genética , RNA Mensageiro/metabolismo , Pequeno RNA não Traduzido/genética , Pequeno RNA não Traduzido/metabolismo
12.
Environ Res ; 243: 117874, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38070852

RESUMO

BACKGROUND: Indoor pollutants have been associated with worse clinical outcomes in chronic obstructive pulmonary disease (COPD). Elevated biomarkers are associated with ambient pollution exposure, however the association with indoor pollution remains unclear. METHODS: Former smokers with spirometry-confirmed COPD were randomized to portable air cleaner or placebo. Indoor particulate matter (PM2.5, PM10, and ultrafine particles [UFP; PM<0.1]) and biomarkers were measured longitudinally at pre-specified intervals and course PM fraction (PM10-2.5) was calculated. Biomarkers were categorized based on associations with biologic mechanisms: inflammation (white blood cell count, interleukin [IL]-6, IL-8, IL-1ß, tumor necrosis factor-α, interferon-γ, serum amyloid A), platelet activation (P-selectin, CD40 ligand [CD40L], 11-dehdydro-thromboxane-B2 [11dTxB2]), endothelial dysfunction (Vascular Cell Adhesion Molecule [VCAM]-1, Intercellular Adhesion Molecule [ICAM]-1), and oxidative stress (thiobarbituric acid reactive substances [TBARS], 8-hydroxydeoxyguanosine, 8-isoprostane). Associations between PM concentrations and each biomarker were analyzed using multivariable linear mixed models. An intention-to-treat analysis was performed to evaluate the air cleaner intervention on the biomarker levels longitudinally. RESULTS: Fifty-eight participants were randomized to each group. Finer PM was more strongly associated with higher IL-8 (mean difference per doubling: UFP 13.9% [p = 0.02], PM2.5 6.8% [p = 0.002], PM10-2.5 5.0% [p = 0.02]) while interferon-γ was associated with UFP and IL-1ß with PM10-2.5. UFP and PM2.5 were associated with elevated levels of the oxidative stress biomarkers TBARS and 8-isoprostane respectively. For platelet activation markers, UFP was associated with higher 11dTxB2 while PM2.5 was associated with higher P-selectin and CD40L. Pollutants were not associated with biomarkers of endothelial dysfunction. In intention-to-treat analysis there was no association of the air cleaner intervention with any of the biomarkers. DISCUSSION: Among former smokers with COPD, elevated levels of indoor air pollutants, particularly ultrafine particles (PM<0.1), were associated with elevated biomarkers of inflammation, platelet activation, and oxidative stress. However, an air cleaner intervention that reduced PM did not significantly reduce biomarker levels.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Poluição do Ar , Doença Pulmonar Obstrutiva Crônica , Humanos , Material Particulado/análise , Selectina-P/análise , Substâncias Reativas com Ácido Tiobarbitúrico/análise , Ligante de CD40/análise , Interferon gama , Interleucina-8/análise , Fumantes , Poluentes Atmosféricos/análise , Biomarcadores , Inflamação/metabolismo , Poluição do Ar/análise , Poluição do Ar em Ambientes Fechados/análise , Exposição Ambiental/análise
13.
Chronic Obstr Pulm Dis ; 11(1): 47-55, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-37931596

RESUMO

Background: Low socioeconomic status (SES) has been associated with worse clinical outcomes in chronic obstructive pulmonary disease (COPD). Food insecurity is more common among individuals with low SES and has been associated with poor outcomes in other chronic illnesses, but its impact on COPD has not been studied. Methods: Former smokers with spirometry-confirmed COPD were recruited from low-income areas of Baltimore, Maryland, and followed for 9 months as part of a cohort study of diet and indoor air pollution. Food insecurity and respiratory outcomes, including COPD exacerbations and patient-reported outcomes, were assessed at regular intervals. The association between food insecurity and COPD outcomes was analyzed using generalized linear mixed models. Additional analyses examined the association of COPD morbidity with subdomains of food insecurity and the association of food insecurity with psychological well-being measures. Results: Ninety-nine participants had available data on food insecurity and COPD outcomes. A total of 26.3% of participants were food insecure at 1 or more times during the study. After adjusting for individual SES, neighborhood poverty, and low healthy food access, food insecurity was associated with a higher incidence rate of moderate and severe exacerbations and worse dyspnea, COPD health status, and respiratory-specific quality of life. Subdomains of food insecurity were independently associated with worse patient-reported outcomes. Food insecurity was additionally associated with higher perceived stress. Discussion: Among former smokers with COPD, food insecurity was associated with a higher incidence of exacerbations, worse patient-reported outcomes, and higher perceived stress. Subdomains of food insecurity were independently associated with worse patient-reported outcomes.

14.
Angew Chem Int Ed Engl ; 63(3): e202316295, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-38057496

RESUMO

Oligomer acceptors in organic solar cells (OSCs) have garnered substantial attention owing to their impressive power conversion efficiency (PCE) and long-term stability. However, the simple and efficient synthesis of oligomer acceptors with higher glass transition temperatures (Tg ) remains a formidable challenge. In this study, we propose an innovative strategy for the synthesis of tetramers, denoted as Tet-n, with elevated Tg s, achieved through only two consecutive Stille coupling reactions. Importantly, our strategy significantly reduces the redundancy in reaction steps compared to conventional methods for linear tetramer synthesis, thereby improving both reaction efficiency and yield. Furthermore, the OSC based on PM6:Tet-1 attains a high PCE of 17.32 %, and the PM6:L8-BO:Tet-1 ternary device achieves an even more higher PCE of 19.31 %. Remarkably, the binary device based on the Tet-1 tetramer demonstrates outstanding operational stability, retaining 80 % of the initial efficiency (T80 ) even after 1706 h of continuous illumination, which is primarily attributed to the enhanced Tg (247 °C) and lower diffusion coefficient (1.56×10-27  cm2 s-1 ). This work demonstrates the effectiveness of our proposed approach in the straightforward and efficient synthesis of tetramers materials with higher Tg s, thus offering a viable pathway for developing high-efficiency and stable OSCs.

15.
Adv Mater ; 36(2): e2307523, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37972308

RESUMO

The development of organic-based optoelectronic technologies for the indoor Internet of Things market, which relies on ambient energy sources, has increased, with organic photovoltaics (OPVs) and photodetectors (OPDs) considered promising candidates for sustainable indoor electronic devices. However, the manufacturing processes of standalone OPVs and OPDs can be complex and costly, resulting in high production costs and limited scalability, thus limiting their use in a wide range of indoor applications. This study uses a multi-component photoactive structure to develop a self-powering dual-functional sensory device with effective energy harvesting and sensing capabilities. The optimized device demonstrates improved free-charge generation yield by quantifying charge carrier dynamics, with a high output power density of over 81 and 76 µW cm-2 for rigid and flexible OPVs under indoor conditions (LED 1000 lx (5200 K)). Furthermore, a single-pixel image sensor is demonstrated as a feasible prototype for practical indoor operating in commercial settings by leveraging the excellent OPD performance with a linear dynamic range of over 130 dB in photovoltaic mode (no external bias). This apparatus with high-performance OPV-OPD characteristics provides a roadmap for further exploration of the potential, which can lead to synergistic effects for practical multifunctional applications in the real world by their mutual relevance.

16.
Small ; 20(12): e2308216, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37946696

RESUMO

The ternary strategy is one of the effective methods to regulate the morphology of the active layer in organic solar cells (OSCs). In this work, the ternary OSCs with bulk heterojunction (BHJ) or layer-by-layer (LbL) active layers are prepared by using the polymer donor PM6 and the non-fullerene acceptor L8-BO as the main system and the fullerene acceptor PC71BM as the third component. The power conversion efficiencies (PCEs) of BHJ OSCs and LbL OSCs are increased from 17.10% to 18.02% and from 17.20% to 18.20% by introducing PC71BM into the binary active layer, respectively. The in situ UV-vis absorption spectra indicate that the molecular aggregation and crystallization process can be prolonged by introducing PC71BM into the PM6:L8-BO or PM6/L8-BO active layer. The molecular orientation and molecular crystallinity in the active layer are optimized by introducing the PC71BM into the binary BHJ or LbL active layers, which can be confirmed by the experimental results of grazing incidence wide-angle X-ray scattering. This study demonstrates that the third component PC71BM can be used as a morphology regulator to regulate the morphology of BHJ or LbL active layers, thus effectively improving the performance of BHJ and LbL OSCs.

17.
Adv Mater ; 36(3): e2305356, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37555531

RESUMO

Most top-rank organic solar cells (OSCs) are manufactured by the halogenated solvent chloroform, which possesses a narrow processing window due to its low-boiling point. Herein, based on two high-boiling solvents, halogenated solvent chlorobenzene (CB) and non-halogenated green solvent ortho-xylene (OX), preparing active layers with the hot solution is put forward to enhance the performance of the OSCs. In situ test and morphological characterization clarify that the hot-casting strategy assists in the fast and synchronous molecular assembly of both donor and acceptor in the active layer, contributing to preferable donor/acceptor ratio, vertical phase separation, and molecular stacking, which is beneficial to charge generation and extraction. Based on the PM6:BO-4Cl, the hot-casting OSCs with a wide processing window achieve efficiencies of 18.03% in CB and 18.12% in OX, which are much higher than the devices processed with room temperature solution. Moreover, the hot-casting devices with PM6:BTP-eC9 deliver a remarkable fill factor of 80.31% and efficiency of 18.52% in OX, representing the record value among binary devices with green solvent. This work demonstrates a facile strategy to manipulate the molecular distribution and arrangement for boosting the efficiency of OSCs with high-boiling solvents.

18.
Adv Mater ; 36(4): e2305416, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37572077

RESUMO

Developing high-performance n-type polymer mixed ionic-electronic conductors (PMIECs) is a grand challenge, which largely determines their applications in vaious organic electronic devices, such as organic electrochemical transistors (OECTs) and organic thermoelectrics (OTEs). Herein, two halogen-functionalized PMIECs f-BTI2g-TVTF and f-BTI2g-TVTCl built from fused bithiophene imide dimer (f-BTI2) as the acceptor unit and halogenated thienylene-vinylene-thienylene (TVT) as the donor co-unit are reported. Compared to the control polymer f-BTI2g-TVT, the fluorinated f-BTI2g-TVTF shows lower-positioned lowest unoccupied molecular orbital (LUMO), improved charge transport property, and greater ion uptake capacity. Consequently, f-BTI2g-TVTF delivers a state-of-the-art µC* of 90.2 F cm-1 V-1 s-1 with a remarkable electron mobility of 0.41 cm2 V-1 s-1 in OECTs and an excellent power factor of 64.2 µW m-1 K-2 in OTEs. An OECT-based inverter amplifier is further demonstrated with voltage gain up to 148 V V-1 , which is among the highest values for OECT inverters. Such results shed light on the impacts of halogen atoms on developing high-performing n-type PMIECs.

19.
Mar Pollut Bull ; 198: 115823, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38039578

RESUMO

This study proposes a deep learning model, U-Net, to improve surface sediment classification using high-resolution unmanned aerial vehicle (UAV) images. We constructed training datasets with UAV images and corresponding labeling data acquired from three field surveys on the Hwangdo tidal flat. The labeling data indicated the distribution of surface sediment types. We compared the performance of the U-Net model trained in various implementation environments, such as surface sediment criteria, input datasets, and classification models. The U-Net trained with five class criteria-derived from previous classification criteria-yielded valid results (overall accuracy:65.6 %). The most accurate results were acquired from trained U-Net with all input datasets; in particular, the tidal channel density caused a significant increase in accuracy. The accuracy of the U-Net was approximately 20 % higher than that of other classification models. These results demonstrate that surface sediment classification using UAV images and the U-Net model is effective.


Assuntos
Aprendizado Profundo , Dispositivos Aéreos não Tripulados
20.
Adv Mater ; 36(1): e2310503, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37961011

RESUMO

High-performance n-type polymeric mixed ionic-electronic conductors (PMIECs) are essential for realizing organic electrochemical transistors (OECTs)-based low-power complementary circuits and biosensors, but their development still remains a great challenge. Herein, by devising two novel n-type polymers (f-BTI2g-SVSCN and f-BSeI2g-SVSCN) containing varying selenophene contents together with their thiophene-based counterpart as the control, it is demonstrated that gradually increasing selenophene loading in polymer backbones can simultaneously yield lowered lowest unoccupied molecular orbital levels, boosted charge-transport properties, and improved ion-uptake capabilities. Therefore, a remarkable volumetric capacitance (C*) of 387.2 F cm-3 and a state-of-the-art OECT electron mobility (µe,OECT ) of 0.48 cm2 V-1 s-1 are synchronously achieved for f-BSeI2g-SVSCN having the highest selenophene content, yielding an unprecedented geometry-normalized transconductance (gm,norm ) of 71.4 S cm-1 and record figure of merit (µC*) value of 191.2 F cm-1 V-1 s-1 for n-type OECTs. Thanks to such excellent performance of f-BSeI2g-SVSCN-based OECTs, a glucose sensor with a remarkably low detection limit of 10 nMm and decent selectivity is further implemented, demonstrating the power of selenophene substitution strategy in enabling high-performance n-type PMIECs for biosensing applications.

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