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1.
Int J Biol Macromol ; 266(Pt 1): 130637, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38490396

RESUMEN

Acute lung injury (ALI) is a prevalent and critical condition in clinical practice. Although certain pharmacological interventions have demonstrated benefits in preclinical studies, none have been proven entirely effective thus far. Therefore, the development of more efficient treatment strategies for ALI is imperative. In this study, we prepared nanostructured lipid carriers (NLCs) conjugated with anti-VCAM-1 antibodies to encapsulate melatonin (MLT), resulting in VCAM/MLT NLCs. This approach aimed to enhance the distribution of melatonin in lung vascular endothelial cells. The VCAM/MLT NLCs had an average diameter of 364 nm, high drug loading content, and a sustained drug release profile. Notably, the NLCs conjugated with anti-VCAM-1 antibodies demonstrated more specific cellular delivery mediated by the VCAM-1 receptors, increased cellular internalization, and enhanced accumulation in lung tissues. Treatment with VCAM/MLT NLCs effectively alleviated pulmonary inflammation by activating NLRP3 inflammasome-dependent pyroptosis through up-regulation of Sirtuin 1. Our findings suggest that VCAM/MLT NLCs demonstrate remarkable therapeutic effects on ALI in both in vitro and in vivo settings, making them a promising and efficient treatment strategy for ALI.


Asunto(s)
Lesión Pulmonar Aguda , Melatonina , Nanoestructuras , Molécula 1 de Adhesión Celular Vascular , Animales , Humanos , Masculino , Ratones , Lesión Pulmonar Aguda/tratamiento farmacológico , Lesión Pulmonar Aguda/metabolismo , Portadores de Fármacos/química , Inflamasomas/metabolismo , Lípidos/química , Melatonina/farmacología , Melatonina/administración & dosificación , Nanoestructuras/química , Proteína con Dominio Pirina 3 de la Familia NLR/metabolismo , Piroptosis/efectos de los fármacos , Transducción de Señal/efectos de los fármacos , Sirtuina 1/metabolismo , Molécula 1 de Adhesión Celular Vascular/metabolismo
2.
Nat Nanotechnol ; 19(6): 775-781, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38429491

RESUMEN

Understanding the mixing behaviour of elements in a multielement material is important to control its structure and property. When the size of a multielement material is decreased to the nanoscale, the miscibility of elements in the nanomaterial often changes from its bulk counterpart. However, there is a lack of comprehensive and quantitative experimental insight into this process. Here we explored how the miscibility of Au and Rh evolves in nanoparticles of sizes varying from 4 to 1 nm and composition changing from 15% Au to 85% Au. We found that the two immiscible elements exhibit a phase-separation-to-alloy transition in nanoparticles with decreased size and become completely miscible in sub-2 nm particles across the entire compositional range. Quantitative electron microscopy analysis and theoretical calculations were used to show that the observed immiscibility-to-miscibility transition is dictated by particle size, composition and possible surface adsorbates present under the synthesis conditions.

3.
J Am Chem Soc ; 146(13): 8971-8980, 2024 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-38393312

RESUMEN

Nonlinear optical (NLO) switching materials, which exhibit reversible intensity modulation in response to thermal stimuli, have found extensive applications across diverse fields including sensing, photoelectronics, and photonic applications. While significant progress has been made in solid-state NLO switching materials, these materials typically showcase their highest NLO performance near room temperature. However, this performance drastically deteriorates upon heating, primarily due to the phase transition undergone by the materials from noncentrosymmetric to centrosymmetric phase. Here, we introduce a new class of NLO switching materials, solid-state supramolecular compounds 18-Crown-6 ether@Cu2Cl4·4H2O (1·4H2O), exhibiting reversible and stable NLO switching when subjected to near-infrared (NIR) photoexcitation and/or thermal stimuli. The reversible crystal structure in response to external stimuli is attributed to the presence of a weakly coordinated bridging water molecule facilitated by hydrogen bonding/chelation interactions between the metal halide and crown-ether supramolecules. We observed an exceptionally high second-harmonic generation (SHG) signal under continuous photoexcitation, even at temperatures exceeding 110 °C. In addition, the bridging water molecules within the complex can be released and recaptured in a fully reversible manner, all without requiring excessive energy input. This feature allows for precise control of SHG signal activation and deactivation through structural transformations, resulting in a high-contrast off/on ratio, reaching values in the million-fold range.

4.
EClinicalMedicine ; 67: 102368, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-38169700

RESUMEN

Background: Stroke and dementia are the leading causes of neurological disease burden. Detrimental effects of air pollution on both conditions are increasingly recognised, while the impacts on the dynamic transitions have not yet been explored, and whether critical time intervals exist is unknown. Methods: This prospective study was conducted based on the UK Biobank. Annual average air pollution concentrations at baseline year 2010 estimated by land-use regression models were used as a proxy for long-term air pollution exposure. Associations between multiple air pollutants (PM2.5, PM2.5-10, and NO2) indicated by air pollution score and the dynamic transitions of stroke and dementia were estimated, and the impacts during critical time intervals were explored. The date cutoff of this study was February 29, 2020. Findings: During a median follow-up of 10.9 years in 413,372 participants, 6484, 3813, and 376 participants developed incident stroke, dementia, and comorbidity of stroke and dementia. For the overall transition from stroke to comorbid dementia, the hazard ratio (HR) for each interquartile range (IQR) increase in air pollution score was 1.38 (95% CI, 1.15, 1.65), and the risks were limited to two time intervals (within 1 year and over 5 years after stroke). As for the transition from dementia to comorbid stroke, increased risk was only observed during 2-3 years after dementia. Interpretation: Our findings suggested that air pollution played an important role in the dynamic transition of stroke and dementia even at concentrations below the current criteria. The findings provided new evidence for alleviating the disease burden of neurological disorders related to air pollution during critical time intervals. Funding: The State Scholarship Fund of China Scholarship Council.

5.
Science ; 383(6678): 86-93, 2024 Jan 05.
Artículo en Inglés | MEDLINE | ID: mdl-38175897

RESUMEN

The metal-halide ionic octahedron is the optoelectronic unit for halide perovskites, and a crown ether-assisted supramolecular assembly approach can pack various ionic octahedra into tunable symmetries. In this work, we demonstrate near-unity photoluminescence quantum yield (PLQY) blue and green emission with the supramolecular assembly of hafnium (Hf) and zirconium (Zr) halide octahedral clusters. (18C6@K)2HfBr6 powders showed blue emission with a near-unity PLQY (96.2%), and green emission was also achieved with (18C6@K)2ZrCl4Br2 powders at a PLQY of 82.7%. These highly emissive powders feature facile low-temperature solution-based synthesis conditions and maintain high PLQY in solution-processable semiconductor inks under ambient conditions, and they were used in thin-film displays and emissive three-dimensional-printed architectures that exhibited high spatial resolution.

6.
Environ Res ; 243: 117825, 2024 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-38081346

RESUMEN

BACKGROUND: Evidence linking ozone to depression and anxiety disorders remains sparse and results are heterogeneous. It remains unknown whether omega-3 fatty acid, or genetic susceptibility of mental disorders modify the impacts of ozone. The aim is to assess the associations of ambient ozone with depression and anxiety, and further explore the potential modification effects of omega-3 fatty acid and genetic susceptibility. METHODS: In total of 257,534 participants were enrolled from 2006 to 2010 and followed up to 2016. Depression and anxiety were assessed using mental health questionnaires, primary care records and hospital admission records. The annual average concentrations of ozone were calculated and linked to individuals by home address. Dietary intake and plasma concentration were selected to reflect levels of omega-3 fatty acid. Polygenetic risk scores were selected to reflect genetic susceptibility. We examined the associations of ozone and incident mental disorders, and potential modification of omega-3 fatty acid and genetic susceptibility. RESULTS: Incidences of depression (N = 6957) and anxiety (N = 6944) was associated with increase of ozone. Higher levels of omega-3 fatty acid might attenuate the ozone related depression risk. However, the modification effects of genetic susceptibility were not found. CONCLUSIONS: Long-term exposure to ambient ozone increase the risk of mental disorders among the middle aged and older adults, and omega-3 fatty acid could reduce the adverse effects of ozone on mental health. Higher intake of omega-3 fatty acid is a potential strategy to prevent the risks caused by ozone on public mental health.


Asunto(s)
Ácidos Grasos Omega-3 , Trastornos Mentales , Ozono , Persona de Mediana Edad , Humanos , Anciano , Ozono/toxicidad , Biobanco del Reino Unido , Bancos de Muestras Biológicas , Trastornos Mentales/inducido químicamente , Trastornos Mentales/epidemiología , Predisposición Genética a la Enfermedad
7.
Sci Total Environ ; 912: 168967, 2024 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-38042194

RESUMEN

BACKGROUND: Stroke and dementia are major neurological disorders that contribute significantly to disease burden and are interlinked in terms of risk. Nevertheless, there is currently no study investigating the influence of residential greenspace on the trajectory of these neurological disorders. METHODS: This longitudinal study utilized data from the UK Biobank. Exposure to residential greenspace was measured by the percentage of total greenspace coverage within a 300-meter buffer zone surrounding the participants' residences. A multistate model was employed to illustrate the trajectory of major neurological disorders, and a piecewise Cox regression model was applied to explore the impact of residential greenspace on different time courses of disease transitions. RESULTS: With 422,649 participants and a median follow-up period of 12.5 years, 8568 (2.0 %), 5648 (1.3 %), and 621 (0.1 %) individuals developed incident stroke, dementia, and comorbidity of both conditions, respectively. An increase in residential greenspace by one interquartile range was associated with reduced risks of transitions from baseline to stroke, dementia, and death, as well as from stroke to comorbidity. The corresponding hazard ratios (HRs) were 0.967 (95 % CI: 0.936, 0.998), 0.928 (0.892, 0.965), 0.925 (0.907, 0.942), and 0.799 (0.685, 0.933), respectively. Furthermore, the protective effect of residential greenspace on the transition from stroke or dementia to comorbidity was particularly pronounced within the first year and over 5 years after stroke and during the 2 to 3 years after dementia onset, with HRs of 0.692 (0.509, 0.941), 0.705 (0.542, 0.918), and 0.567 (0.339, 0.949), respectively. CONCLUSION: This study observed a protective role of residential greenspace in the trajectory of major neurological disorders and contributed to identifying critical progression windows. These findings underscore the significance of environment-health interactions in the prevention of neurological disorders.


Asunto(s)
Demencia , Accidente Cerebrovascular , Humanos , Estudios Longitudinales , Biobanco del Reino Unido , Bancos de Muestras Biológicas , Parques Recreativos , Accidente Cerebrovascular/epidemiología , Demencia/epidemiología
8.
Nano Lett ; 23(24): 11469-11476, 2023 Dec 27.
Artículo en Inglés | MEDLINE | ID: mdl-38060980

RESUMEN

Energy funneling is a phenomenon that has been exploited in optoelectronic devices based on low-dimensional materials to improve their performance. Here, we introduce a new class of two-dimensional semiconductor, characterized by multiple regions of varying thickness in a single confined nanostructure with homogeneous composition. This "noninteger 2D semiconductor" was prepared via the structural transformation of two-octahedron-layer-thick (n = 2) 2D cesium lead bromide perovskite nanosheets; it consisted of a central n = 2 region surrounded by edge-lying n = 3 regions, as imaged by electron microscopy. Thicker noninteger 2D CsPbBr3 nanostructures were obtained as well. These noninteger 2D perovskites formed a laterally coupled quantum well band alignment with virtually no strain at the interface and no dielectric barrier, across which unprecedented intramaterial funneling of the photoexcitation energy was observed from the thin to the thick regions using time-resolved absorption and photoluminescence spectroscopy.

9.
Sci Total Environ ; 902: 166004, 2023 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-37544462

RESUMEN

BACKGROUND: Epidemiologic evidence on whether iron accumulation in brain modified the association between artificial light at night (ALAN) and incident mental disorders is lacking. The authors aims to investigate modification of brain iron deposition on the associations of ALAN with multiple mental disorders in the middle-aged and older adults. METHODS: This prospective study used data from the UK Biobank. ALAN was drawn from satellite datasets. Susceptibility-weighted magnetic resonance imaging was used to ascertain iron content of each brain region. T2* signal loss was used as indices of iron deposition. The main outcomes are impacts of ALAN exposure on onset of wide spectrum of physician-diagnosed mental disorders, which was estimated by time-varying Cox proportional hazard model. The authors further conducted stratified analyses by levels of iron brain deposition to examine the potential modifying effects. RESULTS: Among 298,283 participants followed for a median of 10.91 years, higher ALAN exposure was associated with increased risk of mental disorders. An IQR (11.37 nW/cm2/sr) increase in annual levels of ALAN was associated with an HR of 1.050 (95 % CI: 1.034,1.066) for any mental disorder, 1.076 (95 % CI: 1.053,1.099) for substance use disorder, and 1.036 (95 % CI: 1.004,1.069) for depression disorder in fully adjusted models. The exposure-response curves showed steeper trends at lower ALAN levels and a plateau at higher exposures. The associations were stronger in participants with high iron deposition in left hippocampus, left accumbens and left pallidum. CONCLUSIONS: ALAN was associated with multiple mental disorders in the middle-aged and older adults, and the findings indicated stricter standards of ALAN is needed and targeted preventive measures are warranted, especially with high brain iron deposition.


Asunto(s)
Contaminación Lumínica , Trastornos Mentales , Persona de Mediana Edad , Humanos , Anciano , Incidencia , Estudios Prospectivos , Trastornos Mentales/epidemiología , Imagen por Resonancia Magnética , Encéfalo/diagnóstico por imagen , Luz
10.
Nature ; 621(7978): 282-288, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37587347

RESUMEN

Although high-entropy materials are excellent candidates for a range of functional materials, their formation traditionally requires high-temperature synthetic procedures of over 1,000 °C and complex processing techniques such as hot rolling1-5. One route to address the extreme synthetic requirements for high-entropy materials should involve the design of crystal structures with ionic bonding networks and low cohesive energies. Here we develop room-temperature-solution (20 °C) and low-temperature-solution (80 °C) synthesis procedures for a new class of metal halide perovskite high-entropy semiconductor (HES) single crystals. Due to the soft, ionic lattice nature of metal halide perovskites, these HES single crystals are designed on the cubic Cs2MCl6 (M=Zr4+, Sn4+, Te4+, Hf4+, Re4+, Os4+, Ir4+ or Pt4+) vacancy-ordered double-perovskite structure from the self-assembly of stabilized complexes in multi-element inks, namely free Cs+ cations and five or six different isolated [MCl6]2- anionic octahedral molecules well-mixed in strong hydrochloric acid. The resulting single-phase single crystals span two HES families of five and six elements occupying the M-site as a random alloy in near-equimolar ratios, with the overall Cs2MCl6 crystal structure and stoichiometry maintained. The incorporation of various [MCl6]2- octahedral molecular orbitals disordered across high-entropy five- and six-element Cs2MCl6 single crystals produces complex vibrational and electronic structures with energy transfer interactions between the confined exciton states of the five or six different isolated octahedral molecules.

11.
J Am Chem Soc ; 145(32): 18007-18014, 2023 Aug 16.
Artículo en Inglés | MEDLINE | ID: mdl-37540785

RESUMEN

Achromatic quarter waveplates (A-QWPs), traditionally constructed from multiple birefringent crystals, can modulate light polarization and retardation across a broad range of wavelengths. This mechanism is inherently related to phase retardation controlled by the fast and slow axis of stacked multi-birefringent crystals. However, the conventional design of A-QWPs requires the incorporation of multiple birefringent crystals, which complicates the manufacturing process and raises costs. Here, we report the discovery of a broadband (540-1060 nm) A-QWP based on a two-dimensional (2D) layered hybrid copper halide (HCH) perovskite single crystal. The 2D copper chloride (CuCl6) layers of the HCH crystal undergo Jahn-Teller distortion and subsequently trigger the in-plane optical birefringence. Its broad range of the wavelength response as an A-QWP is a consequence of the out-of-plane mosaicity formed among the stacked inorganic layers during the single-crystal self-assembly process in the solution phase. Given the versatility of 2D hybridhalide perovskites, the 2D HCH crystal offers a promising approach for designing cost-effective A-QWPs and the ability to integrate other optical devices.

12.
J Voice ; 2023 Jul 21.
Artículo en Inglés | MEDLINE | ID: mdl-37482517

RESUMEN

OBJECTIVE: To investigate the morphological changes and motor functions of the larynx in unilateral vocal fold paralysis by using dynamic three-dimensional CT, and to explore the differences between vocal fold paralysis with different nerves involved. METHODS: Twenty-five patients with unilateral vocal fold paralysis and 10 healthy subjects were selected as the paralytic group and the normal group, respectively. Ten dynamic sequence images of laryngeal movement from inhalation to phonation were reviewed, and the glottic morphology at the coronal position, the minimum glottic area at the horizontal position, and the overall activity of the two groups were compared. The 25 patients with unilateral vocal fold paralysis were divided into the thyroarytenoid (TA) muscle group, the TA and posterior cricoarytenoid (PCA) (TA + PCA) muscle group, and the PCA muscle group. The coronal and horizontal parameters of the three types were compared as noted above and the dynamic parameter changes were also compared between the groups. RESULTS: The height and thickness of bilateral vocal cords, the minimum glottic area, and the whole glottic activity were different in the paralysis group and were significantly different from those of the normal group (P < 0.05). The value of the glottic gap ratio and its decrease rate in the TA + PCA group was smaller than those in the TA and PCA group, and the glottic gap ratio was the largest in the PCA group. CONCLUSION: Dynamic CT can provide a qualitative evaluation of laryngeal morphology and quantitative evaluation of motor function in vocal fold paralysis.

13.
Ecotoxicol Environ Saf ; 258: 114992, 2023 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-37167735

RESUMEN

OBJECTIVES: Recent studies have linked exposure to road traffic noise or air pollution with incident type 2 diabetes (T2D), but investigation on their co-exposure was limited and underlying mechanisms remain unclear. We hypothesized that long-term co-exposure to road traffic noise and air pollution increases the risk of incident T2D via the development of metabolic syndrome (MetS). METHODS: This prospective study included 390,834 participants in UK Biobank. Cumulative risk index (CRI), the health-based weighted levels of multiple exposures, was applied to characterize the co-exposure to 24-hour road traffic noise (Lden), particulate matter with aerodynamic diameter ≤ 2.5 µm (PM2.5), and nitrogen dioxide (NO2). Lden was modeled by the Common Noise Assessment Methods in Europe and air pollutant levels were measured by the Land Use Regression model at participants' residential addresses. Incident T2D was ascertained through linkages to inpatient hospital records. MetS was defined by five (central obesity, triglycerides, HDL cholesterol, glucose, and blood pressure) or six factors (C-reactive protein additionally). Cox proportional hazard models were used to assess the association between environmental exposures and incident T2D, and mediation analyses were applied to investigate the role of MetS. RESULTS: After a median of 10.9 years of follow-up, 13,214 (3.4%) incident T2D cases were ascertained. The exposure to Lden, PM2.5, and NO2, as well as their co-exposure, were significantly associated with an elevated risk of incident T2D, with HRs of 1.03 (95%CI: 1.00, 1.05) per 3.5 dB(A) increase in Lden, 1.05 (95%CI: 1.01, 1.10) per 1.3 µg/m3 increase in PM2.5, 1.07 (95%CI: 1.02, 1.11) per 9.8 µg/m3 increase in NO2, and 1.06 (95%CI: 1.02, 1.09) per interquartile range increase in CRI. MetS significantly mediated 43.5%- 54.7% of the CRI-T2D relationship. CONCLUSIONS: Long-term co-exposure to road traffic noise and air pollution is associated with an elevated risk of incident T2D, which may partly be mediated by MetS.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Diabetes Mellitus Tipo 2 , Síndrome Metabólico , Ruido del Transporte , Humanos , Ruido del Transporte/efectos adversos , Síndrome Metabólico/epidemiología , Síndrome Metabólico/etiología , Diabetes Mellitus Tipo 2/epidemiología , Diabetes Mellitus Tipo 2/etiología , Estudios Prospectivos , Dióxido de Nitrógeno/efectos adversos , Dióxido de Nitrógeno/análisis , Contaminación del Aire/efectos adversos , Contaminación del Aire/análisis , Contaminantes Atmosféricos/efectos adversos , Contaminantes Atmosféricos/análisis , Material Particulado/efectos adversos , Material Particulado/análisis , Exposición a Riesgos Ambientales/efectos adversos , Exposición a Riesgos Ambientales/análisis
14.
Environ Res ; 231(Pt 2): 116189, 2023 08 15.
Artículo en Inglés | MEDLINE | ID: mdl-37211178

RESUMEN

BACKGROUND: Intracerebral hemorrhage (ICH) is a subtype of stroke that would cause high mortality and disability. Environmental factors may play an important role in the incident risk of ICH. Evidence on how long-term road traffic noise exposure affects incident ICH is still scarce, and whether green space has a modification effect is unknown. We conducted a prospective analysis based on UK Biobank to assess the longitudinal association between road traffic noise exposure and incident ICH, and the potential modification of green space. METHODS: Algorithms based on medical records and linkage were utilized to identify ICH incident cases in the UK Biobank. The Common Noise Assessment Methods in Europe noise model was used to calculate the road traffic noise exposure at the residential level. The relationship between weighted average 24-h road traffic noise level (Lden) and incident ICH was assessed using Cox proportional hazard models, and the modification effect of green space was examined using stratified analysis with interaction terms. RESULTS: Over a median follow-up of 12.5 years, 1 459 incident ICH cases were ascertained in the 402 268 baseline individuals. After adjustment for potential confounders, Lden was significantly related to an elevated risk of incident ICH with a hazard ratio (HR) of 1.14 (95% CI: 1.01, 1.28) for a 10 dB [A] increment. The detrimental influence of Lden on ICH remained stable after adjustment for air pollution. Furthermore, green space modified the association between Lden exposure and incident ICH (Pinteraction = 0.035), and no association was found for higher green space. CONCLUSIONS: Long-term residential road traffic noise exposure was associated with an increased risk of ICH, but only for those who live in areas with less green space, indicating that green space may alleviate the negative impacts of road traffic noise exposure on ICH.


Asunto(s)
Contaminación del Aire , Ruido del Transporte , Humanos , Ruido del Transporte/efectos adversos , Estudios Prospectivos , Parques Recreativos , Exposición a Riesgos Ambientales/efectos adversos , Exposición a Riesgos Ambientales/análisis , Contaminación del Aire/efectos adversos , Hemorragia Cerebral/epidemiología , Hemorragia Cerebral/etiología
15.
J Am Chem Soc ; 145(18): 10116-10125, 2023 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-37115017

RESUMEN

Silver-copper (AgCu) bimetallic catalysts hold great potential for electrochemical carbon dioxide reduction reaction (CO2RR), which is a promising way to realize the goal of carbon neutrality. Although a wide variety of AgCu catalysts have been developed so far, it is relatively less explored how these AgCu catalysts evolve during CO2RR. The absence of insights into their stability makes the dynamic catalytic sites elusive and hampers the design of AgCu catalysts in a rational manner. Here, we synthesized intermixed and phase-separated AgCu nanoparticles on carbon paper electrodes and investigated their evolution behavior in CO2RR. Our time-sequential electron microscopy and elemental mapping studies show that Cu possesses high mobility in AgCu under CO2RR conditions, which can leach out from the catalysts by migrating to the bimetallic catalyst surface, detaching from the catalysts, and agglomerating as new particles. Besides, Ag and Cu manifest a trend to phase-separate into Cu-rich and Ag-rich grains, regardless of the starting catalyst structure. The composition of the Cu-rich and Ag-rich grains diverges during the reaction and eventually approaches thermodynamic values, i.e., Ag0.88Cu0.12 and Ag0.05Cu0.95. The separation between Ag and Cu has been observed in the bulk and on the surface of the catalysts, highlighting the importance of AgCu phase boundaries for CO2RR. In addition, an operando high-energy-resolution X-ray absorption spectroscopy study confirms the metallic state of Cu in AgCu as the catalytically active sites during CO2RR. Taken together, this work provides a comprehensive understanding of the chemical and structural evolution behavior of AgCu catalysts in CO2RR.

16.
Front Bioeng Biotechnol ; 11: 1175184, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-36970619

RESUMEN

[This corrects the article DOI: 10.3389/fbioe.2022.984424.].

18.
J Am Chem Soc ; 145(8): 4800-4807, 2023 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-36795997

RESUMEN

Halide perovskite is a unique dynamical system, whose structural and chemical processes happening across different timescales have significant impact on its physical properties and device-level performance. However, due to its intrinsic instability, real-time investigation of the structure dynamics of halide perovskite is challenging, which hinders the systematic understanding of the chemical processes in the synthesis, phase transition, and degradation of halide perovskite. Here, we show that atomically thin carbon materials can stabilize ultrathin halide perovskite nanostructures against otherwise detrimental conditions. Moreover, the protective carbon shells enable atomic-level visualization of the vibrational, rotational, and translational movement of halide perovskite unit cells. Albeit atomically thin, protected halide perovskite nanostructures can maintain their structural integrity up to an electron dose rate of 10,000 e-/Å2·s while exhibiting unusual dynamical behaviors pertaining to the lattice anharmonicity and nanoscale confinement. Our work demonstrates an effective method to protect beam-sensitive materials during in situ observation, unlocking new solutions to study new modes of structure dynamics of nanomaterials.

19.
Nature ; 614(7947): 262-269, 2023 02.
Artículo en Inglés | MEDLINE | ID: mdl-36755171

RESUMEN

Carbon dioxide electroreduction facilitates the sustainable synthesis of fuels and chemicals1. Although Cu enables CO2-to-multicarbon product (C2+) conversion, the nature of the active sites under operating conditions remains elusive2. Importantly, identifying active sites of high-performance Cu nanocatalysts necessitates nanoscale, time-resolved operando techniques3-5. Here, we present a comprehensive investigation of the structural dynamics during the life cycle of Cu nanocatalysts. A 7 nm Cu nanoparticle ensemble evolves into metallic Cu nanograins during electrolysis before complete oxidation to single-crystal Cu2O nanocubes following post-electrolysis air exposure. Operando analytical and four-dimensional electrochemical liquid-cell scanning transmission electron microscopy shows the presence of metallic Cu nanograins under CO2 reduction conditions. Correlated high-energy-resolution time-resolved X-ray spectroscopy suggests that metallic Cu, rich in nanograin boundaries, supports undercoordinated active sites for C-C coupling. Quantitative structure-activity correlation shows that a higher fraction of metallic Cu nanograins leads to higher C2+ selectivity. A 7 nm Cu nanoparticle ensemble, with a unity fraction of active Cu nanograins, exhibits sixfold higher C2+ selectivity than the 18 nm counterpart with one-third of active Cu nanograins. The correlation of multimodal operando techniques serves as a powerful platform to advance our fundamental understanding of the complex structural evolution of nanocatalysts under electrochemical conditions.

20.
Artículo en Inglés | MEDLINE | ID: mdl-36833923

RESUMEN

Temperature is increasingly understood to impact mental health. However, evidence of the long-term effect of temperature exposure on the risk of depressive symptoms is still scarce. Based on the China Health and Retirement Longitudinal Study (CHARLS), this study estimated associations between long-term apparent temperature, extreme temperature, and depressive symptoms in middle-aged and older adults. Results showed that a 1 °C increase or decrease from optimum apparent temperature (12.72 °C) was associated with a 2.7% (95% CI: 1.3%, 4.1%) and 2.3% (95% CI: 1.1%, 3.5%) increased risk of depressive symptoms, respectively. This study also found that each percent increase in annual change in ice days, cool nights, cool days, cold spell durations, and tropical nights was associated with higher risk of depressive symptoms, with HRs (95%CI) of 1.289 (1.114-1.491), 2.064 (1.507-2.825), 1.315 (1.061-1.631), 1.645 (1.306-2.072), and 1.344 (1.127-1.602), respectively. The results also indicated that people living in northern China have attenuated risk of low apparent temperature. Older people were also observed at higher risk relating to more cool nights. Middle-aged people, rural residents, and people with lower household income might have higher related risk of depressive symptoms due to increased tropical nights. Given the dual effect of climate change and global aging, these findings have great significance for policy making and adaptive strategies for long-term temperature and extreme temperature exposure.


Asunto(s)
Depresión , Jubilación , Persona de Mediana Edad , Humanos , Anciano , Estudios Longitudinales , Depresión/psicología , Temperatura , Jubilación/psicología , China
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