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1.
J Am Chem Soc ; 146(10): 6893-6904, 2024 Mar 13.
Article in English | MEDLINE | ID: mdl-38426856

ABSTRACT

Owing to the electrical conductivity and periodic porosity, conductive metal-organic framework (cMOF) ultrathin films open new perspectives to photocatalysis. The space-selective assembly of catalytic sites and photosensitizers in/on cMOF is favorable for promoting the separation of photogenerated carriers and mass transfer. However, the controllable integration of functional units into the cMOF film is rarely reported. Herein, via the synergistic effect of steric hindrance and an electrostatic-driven strategy, the dinuclear-metal molecular catalysts (DMC) and perovskite (PVK) quantum dot photosensitizers were immobilized into channels and onto the surface of cMOF ultrathin films, respectively, affording [DMC@cMOF]-PVK film photocatalysts. In this unique heterostructure, cMOF not only facilitated the charge transfer from PVK to DMC but also guaranteed mass transfer. Using H2O as an electron donor, [DMC@cMOF]-PVK realized a 133.36 µmol·g-1·h-1 CO yield in photocatalytic CO2 reduction, much higher than PVK and DMC-PVK. Owing to the excellent light transmission of films, multilayers of [DMC@cMOF]-PVK were integrated to increase the CO yield per unit area, and the 10-layer device realized a 1115.92 µmol·m-2 CO yield in 4 h, which was 8-fold higher than that of powder counterpart. This work not only lightens the development of cMOF-based composite films but also paves a novel avenue for an ultrathin film photocatalyst.

2.
J Transl Med ; 22(1): 65, 2024 01 16.
Article in English | MEDLINE | ID: mdl-38229122

ABSTRACT

BACKGROUND: Accurate clinical structural variant (SV) calling is essential for cancer target identification and diagnosis but has been historically challenging due to the lack of ground truth for clinical specimens. Meanwhile, reduced clinical-testing cost is the key to the widespread clinical utility. METHODS: We analyzed massive data from tumor samples of 476 patients and developed a computational framework for accurate and cost-effective detection of clinically-relevant SVs. In addition, standard materials and classical experiments including immunohistochemistry and/or fluorescence in situ hybridization were used to validate the developed computational framework. RESULTS: We systematically evaluated the common algorithms for SV detection and established an expert-reviewed SV call set of 1,303 tumor-specific SVs with high-evidence levels. Moreover, we developed a random-forest-based decision model to improve the true positive of SVs. To independently validate the tailored 'two-step' strategy, we utilized standard materials and classical experiments. The accuracy of the model was over 90% (92-99.78%) for all types of data. CONCLUSION: Our study provides a valuable resource and an actionable guide to improve cancer-specific SV detection accuracy and clinical applicability.


Subject(s)
Genomics , Neoplasms , Humans , Benchmarking , Cost-Benefit Analysis , In Situ Hybridization, Fluorescence , Neoplasms/diagnosis , Neoplasms/genetics , Genome, Human , High-Throughput Nucleotide Sequencing
3.
Chem Soc Rev ; 52(4): 1331-1381, 2023 Feb 20.
Article in English | MEDLINE | ID: mdl-36723084

ABSTRACT

Organic semiconductors have received broad attention and research interest due to their unique integration of semiconducting properties with structural tunability, intrinsic flexibiltiy and low cost. In order to meet the requirements of organic electronic devices and their integrated circuits, p-type, n-type and ambipolar organic semiconductors are all necessary. However, due to the limitation in both material synthesis and device fabrication, the development of n-type and ambipolar materials is quite behind that of p-type materials. Recent development in synthetic methods of organic semiconductors greatly enriches the range of n-type and ambipolar materials. Moreover, the newly developed materials with multiple functions also put forward multi-functional device applications, including some emerging research areas. In this review, we give a timely summary on these impressive advances in n-type and ambipolar organic semiconductors with a special focus on their synthesis methods and advanced materials with enhanced properties of charge carrier mobility, integration of high mobility and strong emission and thermoelectric properties. Finally, multi-functional device applications are further demonstrated as an example of these developed n-type and ambipolar materials.

4.
Angew Chem Int Ed Engl ; 63(27): e202402693, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38586976

ABSTRACT

As an effective method to modulate the physicochemical properties of materials, crystal phase engineering, especially hetero-phase, plays an important role in developing high-performance photocatalysts. However, it is still a huge challenge but significant to construct porous hetero-phase nanostructures with adjustable band structures. As a kind of unique porous crystalline materials, metal-organic frameworks (MOFs) might be the appropriate candidate, but the MOF-based hetero-phase is rarely reported. Herein, we developed a secondary building unit (SBU) regulating strategy to prepare two crystal phases of Ti-MOFs constructed by titanium and 1,4-dicarboxybenzene, i.e., COK and MIL-125. Besides, COK/MIL-125 hetero-phase was further constructed. In the photocatalytic hydrogen evolution reaction, COK/MIL-125 possessed the highest H2 yield compared to COK and MIL-125, ascribing to the Z-Scheme homojunction at hetero-phase interface. Furthermore, by decorating with amino groups (i.e., NH2-COK/NH2-MIL-125), the light absorbing capacity was broadened to visible-light region, and the visible-light-driven H2 yield was greatly improved. Briefly, the MOF-based hetero-phase possesses periodic channel structures and molecularly adjustable band structures, which is scarce in traditional organic or inorganic materials. As a proof of concept, our work not only highlights the development of MOF-based hetero-phase nanostructures, but also paves a novel avenue for designing high-performance photocatalysts.

5.
Angew Chem Int Ed Engl ; 63(11): e202319380, 2024 Mar 11.
Article in English | MEDLINE | ID: mdl-38246876

ABSTRACT

Organic light-emitting transistors (OLETs) are highly integrated and minimized optoelectronic devices with significant potential superiority in smart displays and optical communications. To realize these various applications, it is urgently needed for color-tunable emission in OLETs, but remains a great challenge as a result of the difficulty for designing organic semiconductors simultaneously integrating high carrier mobility, strong solid-state emission, and the ability for potential tunable colors. Herein, a high mobility emissive excimer organic semiconductor, 2,7-di(2-anthryl)-9H-fluorene (2,7-DAF) was reasonably designed by introducing a rotatable carbon-carbon single bond connecting two anthracene groups at the 2,7-sites of fluorene, and the small torsion angles simultaneously guarantee effective conjugation and suppress fluorescence quenching. Indeed, the unique stable dimer arrangement and herringbone packing mode of 2,7-DAF single crystal enables its superior integrated optoelectronic properties with high carrier mobility of 2.16 cm2 ⋅ V-1 ⋅ s-1 , and strong excimer emission with absolute photoluminescence quantum yield (PLQY) of 47.4 %. Furthermore, the voltage-dependent electrically induced color-tunable emission from orange to blue was also demonstrated for an individual 2,7-DAF single crystal based OLETs for the first time. This work opens the door for a new class of high mobility emissive excimer organic semiconductors, and provides a good platform for the study of color-tunable OLETs.

6.
Am J Gastroenterol ; 2023 Oct 09.
Article in English | MEDLINE | ID: mdl-37737674

ABSTRACT

INTRODUCTION: Diet is a modifiable metabolic dysfunction-associated steatotic liver disease (MASLD) risk factor, but few studies have been conducted among Hispanic patients, despite the fact that MASLD prevalence and severity are highest among this ethnic subgroup. We aimed to identify prevalent dietary patterns among Hispanic patients using cluster analysis and to investigate associations with MASLD severity. METHODS: This cross-sectional analysis included 421 Harris County MASLD Cohort participants who self-reported Hispanic ethnicity and completed baseline food frequency questionnaires. All included patients had MASLD, diagnosed per standard clinical criteria. K-means analysis was used to identify clusters of patients sharing similar dietary habits. Multivariable adjusted logistic regression was used to estimate associations of dietary clusters with aminotransferases among the overall sample and with histologic steatosis, metabolic dysfunction-associated steatohepatitis, and fibrosis among a subsample of patients who underwent liver biopsy within 6 months of their baseline food frequency questionnaire (n = 186). RESULTS: We identified 2 clusters: a plant-food/prudent and a fast-food/meat pattern. The fast-food/meat pattern was associated with 2.47-fold increased odds (95% confidence interval 1.31-4.65) of more severe steatosis than the plant-food/prudent pattern after adjusting for demographics, metabolic score, physical activity, and alcohol ( q = 0.0159). No significant association was observed between diet and aminotransferases, metabolic dysfunction-associated steatohepatitis, or fibrosis. DISCUSSION: Given the importance of sociocultural influences on diet, it is important to understand dietary patterns prevalent among Hispanic patients with MASLD. Using cluster analysis, we identified 1 plant-based pattern vs 1 distinct fast-food/meat-based pattern associated with detrimental effects among our population. This information is an important starting point for tailoring dietary interventions for Hispanic patients with MASLD.

7.
Cell Commun Signal ; 21(1): 99, 2023 05 04.
Article in English | MEDLINE | ID: mdl-37143083

ABSTRACT

BACKGROUND: Chemotherapy-induced peripheral neuropathy (CIPN) is a serious side effect of chemotherapy with poorly understood mechanisms and few treatments. High-mobility group box 1 (HMGB1)-induced neuroinflammation is the main cause of CIPN. Here, we aimed to illustrate the role of the macrophage scavenger receptor A1 (SR-A1) in HMGB1 clearance and CIPN resolution. METHODS: Oxaliplatin (L-OHP) was used to establish a CIPN model. Recombinant HMGB1 (rHMGB1) (his tag) was used to evaluate the phagocytosis of HMGB1 by macrophages. RESULTS: In the clinic, HMGB1 expression and MMP-9 activity were increased in the plasma of patients with CIPN. Plasma HMGB1 expression was positively correlated with the cumulative dose of L-OHP and the visual analog scale. In vitro, engulfment and degradation of rHMGB1 increased and inflammatory factor expression decreased after AMP-activated protein kinase (AMPK) activation. Neutralizing antibodies, inhibitors, or knockout of SR-A1 abolished the effects of AMPK activation on rHMGB1 engulfment. In vivo, AMPK activation increased SR-A1 expression in the dorsal root ganglion, decreased plasma HMGB1 expression and MMP-9 activity, and attenuated CIPN, which was abolished by AMPK inhibition or SR-A1 knockout in the CIPN mice model. CONCLUSION: Activation of the AMPK/SR-A1 axis alleviated CIPN by increasing macrophage-mediated HMGB1 engulfment and degradation. Therefore, promoting HMGB1 clearance may be a potential treatment strategy for CIPN. Video abstract.


Subject(s)
Antineoplastic Agents , HMGB1 Protein , Peripheral Nervous System Diseases , Mice , Animals , AMP-Activated Protein Kinases , HMGB1 Protein/metabolism , Matrix Metalloproteinase 9 , Oxaliplatin/adverse effects , Peripheral Nervous System Diseases/chemically induced , Peripheral Nervous System Diseases/drug therapy , Antineoplastic Agents/therapeutic use , Receptors, Scavenger/therapeutic use
8.
Langmuir ; 39(35): 12324-12335, 2023 Sep 05.
Article in English | MEDLINE | ID: mdl-37615087

ABSTRACT

The dazzling adsorbent products make people overlook the harm of heavy metals adsorbed on them. Hazardous waste adsorbents cause secondary pollution. In this study, waste lignocellulose was dissolved by alkaline urea solvent and high-intensity ultrasound, then cross-linked by epichlorohydrin to make hydrogel, which was utilized to adsorb toxic heavy-metal wastewater. In situ deposition and high-temperature carbonization turn the gel that has absorbed heavy metals into carbon aerogel-loaded metal oxide energy storage materials that may be employed as anodes in lithium-ion batteries with excellent electrochemical performance. The best reversible capacity was 435.86 mAh g-1 after 100 cycles at 0.2C, indicating that the hazardous solid waste generated by the removal of heavy metals using biomass-based adsorbent has potential lithium battery applications. Thus, we provide a fresh perspective on the efficient recycling of heavy metals as well as an environmentally friendly, high-value conservation strategy for lowering the danger of heavy-metal hazardous wastes.

9.
Phys Chem Chem Phys ; 25(35): 23819-23828, 2023 Sep 13.
Article in English | MEDLINE | ID: mdl-37624427

ABSTRACT

Two-dimensional (2D) phosphorus-rich phosphides generally preserve the excellent electronic properties of phosphorene, making them promising photocatalysts for water splitting. Despite tremendous efforts in the search for potential photocatalysts in 2D phosphides, few known 2D phosphides fully meet the requirements for photocatalytic water splitting. Herein, we systemically investigate a set of penta-MP5 (M = B, Al, Ga, and In) monolayers by first-principles calculations and identify them as potential photocatalysts for water splitting. These penta-MP5 monolayers are found to feature favorable bandgaps of about 2.70 eV with appropriate band edge positions, a high carrier mobility of 1 × 104 cm-2 V-1 s-1, an excellent optical absorption coefficient (OAC) of 1 × 105 cm-1, and a good solar-to-hydrogen (STH) efficiency of 8%. Meanwhile, free energy calculations indicate that these penta-MP5 monolayers present both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) photocatalytic activities under light conditions. All these excellent properties demonstrate that penta-MP5 monolayers are suitable candidates as photocatalysts for promising applications in overall water splitting.

10.
Support Care Cancer ; 31(12): 671, 2023 Nov 04.
Article in English | MEDLINE | ID: mdl-37924363

ABSTRACT

OBJECTIVE: Oncogenic alternation in RET is one of the important targets of non-small cell lung cancer (NSCLC). Pralsetinib has shown great efficacy in RET fusion-positive NSCLC, but a series of adverse reactions will inevitably occur in the meantime. We aimed to explore the clinical characteristics of patients with pneumonia and recognition it in early stage, so patients could longer benefit from pralsetinib. METHODS: This is a multicenter, retrospective study. RET fusion-positive advanced NSCLC patients who developed pneumonia during pralsetinib treatment from January 2020 to December 2022 were included. Clinical data, time to onset of pneumonia, methods of pneumonia diagnosis, treatment with pneumonia, prognosis of pneumonia, and the effect of pneumonia on the efficacy of pralsetinib. RESULTS: A total of 8 patients with pneumonia were included in the study, most of which were non-smoking female patients and the main fusion gene was KIF5B (87.5%), which was consistent with the general characteristics of RET fusion population. The median occurrence time of pralsetinib-associated pneumonia was 2.15 (range 1.1-6.63) months. All patients were infected by opportunistic pathogens, and the most common pathogen was human herpesviruses and pneumospora yerbii. Fever was always the first symptom, and timely anti-infective treatment including antibiotics, antiviral drugs, and antifungal drugs was effective. Until February 28, 2023, the median follow-up time was 18.7 months, the mean PFS of patients was 17.4 months, and the median PFS was not reached. Fortunately, patients who restarted pralsetinib after infection control continued to benefit. CONCLUSIONS: Opportunistic infection may be a unique adverse effect of pralsetinib. During the treatment of pralsetinib, we should be vigilant about the occurrence of pneumonia and achieve early recognition and timely treatment.


Subject(s)
Carcinoma, Non-Small-Cell Lung , Lung Neoplasms , Humans , Female , Carcinoma, Non-Small-Cell Lung/drug therapy , Lung Neoplasms/drug therapy , Lung Neoplasms/genetics , Retrospective Studies , Pyridines/therapeutic use , Proto-Oncogene Proteins c-ret/genetics , Proto-Oncogene Proteins c-ret/therapeutic use
11.
Ethn Health ; 28(2): 299-312, 2023 02.
Article in English | MEDLINE | ID: mdl-35067116

ABSTRACT

OBJECTIVES: Non-alcoholic fatty liver disease (NAFLD) is a highly prevalent liver disease, with the highest prevalence observed in the U.S. among Hispanic/Latino adults. While physical activity and dietary behaviors have established protective associations with NAFLD and its severity, these associations have not been well-characterized in Hispanic/Latino adults. The purpose of this study was to assess the association of lifestyle behaviors with NAFLD and advanced fibrosis in US Hispanic/Latino adults. DESIGN: We selected all Hispanic/Latino adults from the 2017-2018 National Health and Nutrition Examination Survey (NHANES). NAFLD was defined as CAP ≥285 dB/m, and advanced fibrosis as liver stiffness measurements ≥8.6 kPa. Multivariate-adjusted logistic regression models assessed associations of physical activity and sedentary behavior (Global Physical Activity Questionnaire), as well as diet quality (Healthy Eating Index [HEI]-2015) and total energy intake (24-hour recall) with NAFLD and advanced fibrosis. RESULTS: In Hispanic/Latino adults, the overall prevalence of NAFLD was 41.5%, while the prevalence of advanced fibrosis among those with NAFLD was 17.2%. We found that higher levels of physical activity and high diet quality were associated with lower risk of NAFLD. Compared to those reporting on average 0 metabolic equivalent (MET) hours/week of physical activity, participants reporting high levels of physical activity (≥32 MET hours/week) had 40% lower risk of NAFLD (Adjusted OR = 0.60, 95%CI 0.38, 0.93). High diet quality (HEI-2015) was associated with a 30% lower risk of NAFLD (Adjusted OR = 0.70, 95% CI 0.51, 0.97) and 72% lower risk of advanced fibrosis (Adjusted OR = 0.28, 95% CI 0.12, 0.66), as compared to those with low diet quality. CONCLUSIONS: In this population-based study, high levels of physical activity and diet quality were associated with lower risk of NAFLD in Hispanic/Latino adults. Public health and medical professionals need to concentrate efforts on lifestyle behavior change in Hispanic/Latino adults who are at high risk for serious liver disease.


Subject(s)
Hispanic or Latino , Life Style , Non-alcoholic Fatty Liver Disease , Humans , Elasticity Imaging Techniques , Fibrosis , Non-alcoholic Fatty Liver Disease/epidemiology , Non-alcoholic Fatty Liver Disease/complications , Non-alcoholic Fatty Liver Disease/metabolism , Nutrition Surveys , Prevalence , United States
12.
Sensors (Basel) ; 23(16)2023 Aug 18.
Article in English | MEDLINE | ID: mdl-37631782

ABSTRACT

This paper proposed a circular flexible spherical joint to reduce the processing difficulty and manufacturing cost, and design a six-dimensional force sensor based on it. This paper analyzes the influence of the structural parameters of the flexible spherical joints on the accuracy of the six-dimensional force sensor by comparing the force mapping matrix of flexible spherical and ideal spherical joints. As the force mapping matrix is related to the stiffness matrix, the stiffness matrix of a six-dimensional force sensor based on a circular flexible spherical joint and the force mapping matrix of the generalized external force acting on the sensor was derived. Finally, a set of optimal parameters was selected to create a prototype and was verified through finite elements and experiments. The results show that the six-dimensional force sensor with a circular flexible spherical joint has good accuracy and provides some guidance for the design and analysis of the sensor.

13.
Prev Med ; 154: 106903, 2022 01.
Article in English | MEDLINE | ID: mdl-34861339

ABSTRACT

The association of physical activity (PA) and diet quality with non-alcoholic fatty liver disease (NAFLD) and NAFLD-related fibrosis have never been examined in a representative sample of U.S. adults using a more precise form of measuring NAFLD. The purpose of this study was to assess the associations of PA and diet quality (Healthy Eating Index [HEI]-2015) with NAFLD and a subset with advanced fibrosis (F3-4) as assessed by vibration-controlled transient elastography with controlled attenuation parameter in a representative sample of U.S. adults. This cross-sectional analysis uses data from 2017-2018 National Health and Nutrition Examination Survey. NAFLD was defined as controlled attenuation parameter ≥285 dB/m, and high likelihood of advanced fibrosis as liver stiffness measurements ≥8.6 kPa. Associations of HEI-2015 from 24-h dietary recalls and self-reported PA and sedentary behavior were estimated in multivariable-adjusted logistic regression models of NAFLD and advanced fibrosis. In 2892 adults, the prevalence of NAFLD and advanced fibrosis was 35.6% and 5.6%, respectively. We found that high adherence to U.S. dietary recommendations (highest vs. lowest HEI-2015 tertile) and more PA (middle tertile vs. lowest) were associated with reduced odds of NAFLD (Adjusted OR and 95% CI; 0.60 (0.44, 0.84) and 0.65 (0.42, 0.99), respectively). More PA was inversely associated with advanced fibrosis (Adjusted OR = 0.35, 95%CI 0.16, 0.75). Diet quality and PA are associated with reduced odds of NAFLD, and PA may be critical even for those with advanced liver disease. These behaviors should be the focus of targeted public health interventions.


Subject(s)
Non-alcoholic Fatty Liver Disease , Adult , Cross-Sectional Studies , Diet , Exercise , Fibrosis , Humans , Liver Cirrhosis/complications , Liver Cirrhosis/diagnosis , Liver Cirrhosis/epidemiology , Non-alcoholic Fatty Liver Disease/epidemiology , Nutrition Surveys
14.
J Sep Sci ; 45(15): 3043-3053, 2022 Aug.
Article in English | MEDLINE | ID: mdl-35621260

ABSTRACT

A rapid method for determination of parabens preservatives (methyl paraben, ethyl paraben, isopropyl paraben, propyl paraben, isobutyl paraben, and butyl paraben) in flavors was established by using supercritical fluid chromatography-tandem mass spectrometry combined with dispersive solid-phase extraction. After adding methanol and primary secondary amine to the sample simultaneously, high extraction efficiency and good sample cleanup could be obtained by simple shaking. Parabens were well separated on a Chiralpak IG-3 column in 6 min by gradient elution. Recoveries from spiked blank samples at 0.5, 1.0, and 5.0 mg/kg were determined to be 88.3-106.6%with relative standard deviations less than 8.0%. All analytes achieved good linear relation (r ≥ 0.999 2). The limits of detection for all analytes ranged from 0.03 to 0.09 mg/kg and the limits of quantification from 0.11 to 0.31 mg/kg, respectively. A total of 20 actual samples were successfully analyzed by taking the proposed method. Being simple, rapid, green, and reliable, this method can be taken for the determination of parabens preservatives in flavors.


Subject(s)
Chromatography, Supercritical Fluid , Parabens , Chromatography, High Pressure Liquid/methods , Parabens/analysis , Preservatives, Pharmaceutical/analysis , Solid Phase Extraction/methods , Tandem Mass Spectrometry/methods
15.
Immun Ageing ; 19(1): 34, 2022 Jul 25.
Article in English | MEDLINE | ID: mdl-35879802

ABSTRACT

BACKGROUND: The immune cell compartment of the mammalian brain changes dramatically and peripheral T cells infiltrate the brain parenchyma during normal aging. However, the mechanisms underlying age-related T cell infiltration in the central nervous system remain unclear. RESULTS: Chronic inflammation and peripheral T cell infiltration were observed in the subventricular zone of aged mice. Cell-cell interaction analysis revealed that aged microglia released CCL3 to recruit peripheral CD8+ memory T cells. Moreover, the aged microglia shifted towards a pro-inflammation state and released TNF-α to upregulate the expression of VCAM1 and ICAM1 in brain venous endothelial cells, which promoted the transendothelial migration of peripheral T cells. In vitro experiment reveals that human microglia would also transit to a chemotactic phenotype when treated with CSF from the elderly. CONCLUSIONS: Our research demonstrated that microglia play an important role in the aging process of brain by shifting towards a pro-inflammation and chemotactic state. Aged microglia promote T cell infiltration by releasing chemokines and upregulating adhesion molecules on venous brain endothelial cells.

16.
J Soc Pers Relat ; 39(11): 3252-3274, 2022 Nov.
Article in English | MEDLINE | ID: mdl-38603302

ABSTRACT

The COVID-19 pandemic's global scope and resulting social distancing measures have caused unprecedented economic, lifestyle, and social impacts to personal and relationship well-being. While lockdowns have prompted individuals to increase reliance on intimate partners for support, stressful external contexts can also interfere with partners' capacity to request and provide support, resulting in relationship dissatisfaction and even dissolution. Guided by a risk and resilience framework, this study examined the impact of perceived stress, social contextual factors, and dyadic coping on self-reported relationship satisfaction changes during the initial United States COVID-19 lockdown period. Participants were adults in romantic relationships who completed an online survey between April 13 and June 8, 2020. Overall, survey respondents (N = 1106) reported higher perceived stress levels than established population norms, and small but significant decrements in relationship satisfaction. Multivariable models revealed that higher perceived stress levels were associated with lower relationship satisfaction levels. Additionally, dyadic coping was found to moderate the impact of perceived stress on relationship satisfaction (B = .05, 95% CI = .02- .07), suggesting that engaging in dyadic coping buffered individuals from adverse effects of perceived stress on their relationships. Findings emphasize heightened stress experienced by individuals during the pandemic, potential detrimental effects of stress on couple relationships, and suggest dyadic coping may help buffer couples from adverse effects of the pandemic on their relationships. As such, dyadic coping may be an important target for future interventions designed to assist couples during the ongoing pandemic and future pandemics/natural disasters.

17.
Angew Chem Int Ed Engl ; 61(25): e202200791, 2022 Jun 20.
Article in English | MEDLINE | ID: mdl-35298062

ABSTRACT

Integrating high charge-carrier mobility and low-threshold lasing action in an organic semiconductor is crucial for the realization of an electrically pumped laser, but remains a great challenge. Herein, we present an organic semiconductor, named as 2,7-di(2-naphthyl)-9H-fluorene (LD-2), which shows an unexpected high charge-carrier mobility of 2.7 cm2  V-1 s-1 and low-threshold lasing characteristic of 9.43 µJ cm-2 and 9.93 µJ cm-2 and high-quality factor (Q) of 2131 and 1684 at emission peaks of 420 and 443 nm, respectively. Detailed theoretical calculations and photophysical data analysis demonstrate that a large intermolecular transfer integral of 10.36-45.16 meV together with a fast radiative transition rate of 8.0×108  s-1 are responsible for the achievement of the superior integrated optoelectronic properties in the LD-2 crystal. These optoelectronic performances of LD-2 are among the highest reported low-threshold lasing organic semiconductors with efficient charge transport, suggesting its promise for research of electrically pumped organic lasers (EPOLs).

18.
Angew Chem Int Ed Engl ; 61(45): e202206825, 2022 Nov 07.
Article in English | MEDLINE | ID: mdl-35989244

ABSTRACT

Organic semiconductors with combinative high carrier mobility and efficient solid-state emission are full of challenges but urgently pursued for developing new emerging optoelectronics. Herein, by delicately regulating the crystal packing of an anthracene-based molecular crystal via terminal tert-butylation, we developed a superior high mobility emissive molecule, 2,6-di(6-tert-butylnaphthyl)anthracene (TBU-DNA). The unique "slipped herringbone" packing motif of TBU-DNA enables its appropriate exciton-exciton coupling and electron-phonon coupling, thus resulting in remarkably high solid-state emission (photoluminescence quantum yield, ΦF ≈74.9 %) and efficacious charge transport (carrier mobility, µ=5.0 cm2 V-1 s-1 ). Furthermore, OLETs based on TBU-DNA show an external quantum efficiency (EQE) of 1.8 %, which is among the highest EQE values for single component OLETs reported till now. This work presents a crystal engineering strategy via exquisite molecular design to realize high mobility emissive organic semiconductors.

19.
J Am Chem Soc ; 143(46): 19243-19256, 2021 11 24.
Article in English | MEDLINE | ID: mdl-34730972

ABSTRACT

Organic cocrystal engineering refers to two or more organic molecules stoichiometrically combined and held together by noncovalent intermolecular interactions, which differs from standard chemical synthesis involving covalent bond breakage and formation. Organic cocrystals have unique properties and offer a new strategy for creating enhanced organics. First, however, some key questions need to be addressed: How do diverse monomers affect the intermolecular interaction kinetics during cocrystallization? How do the intermolecular forces in cocrystals affect cocrystal functions? In this Perspective, the definition and advantages of organic cocrystal engineering, specifically in the construction of a reliable intermolecular interaction-stacking structure-performance relationship, are outlined. Additionally, recent developments in the field and the questions above are discussed. Finally, a brief conclusion and some hints on likely future developments are provided.

20.
J Am Chem Soc ; 143(42): 17526-17534, 2021 Oct 27.
Article in English | MEDLINE | ID: mdl-34644063

ABSTRACT

At the gas-liquid interface, the confined synthesis of metal-organic framework (MOF) films has been extensively developed by spreading an ultrathin oil layer on the aqueous surface as a reactor. However, this interface is susceptible to various disturbances and incapable of synthesizing large-area crystalline MOF films. Herein, we developed a polymer-assisted space-confined strategy to synthesize large-area films by blending poly(methyl methacrylate) (PMMA) into the oil layer, which improved the stability of the gas-liquid interface and the self-shrinkage of the oil layer on the water surface. Meanwhile, the as-synthesized MOFs as a quasi-solid substrate immobilized the edge of the oil layer, which maintained a large spreading area. Thanks to this synergistic effect, we synthesized the freestanding MOF-based film with a foot-level (0.66 ft) lateral dimension, which is the largest size reported so far. Besides, due to the phase separation of the two components, the MOF-PMMA composite film combined the conductivity of MOFs (1.13 S/m) with the flexibility of PMMA and exhibited excellent mechanical properties. More importantly, this strategy could be extended to the preparation of other MOFs, coordination polymers (CPs), and even inorganic material composite films, bringing light to the design and large-scale synthesis of various composite films for practical applications.

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