Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 53
Filtrar
Más filtros

Banco de datos
País/Región como asunto
Tipo del documento
Intervalo de año de publicación
1.
Nature ; 618(7967): 967-973, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-37380694

RESUMEN

Observational evidence shows the ubiquitous presence of ocean-emitted short-lived halogens in the global atmosphere1-3. Natural emissions of these chemical compounds have been anthropogenically amplified since pre-industrial times4-6, while, in addition, anthropogenic short-lived halocarbons are currently being emitted to the atmosphere7,8. Despite their widespread distribution in the atmosphere, the combined impact of these species on Earth's radiative balance remains unknown. Here we show that short-lived halogens exert a substantial indirect cooling effect at present (-0.13 ± 0.03 watts per square metre) that arises from halogen-mediated radiative perturbations of ozone (-0.24 ± 0.02 watts per square metre), compensated by those from methane (+0.09 ± 0.01 watts per square metre), aerosols (+0.03 ± 0.01 watts per square metre) and stratospheric water vapour (+0.011 ± 0.001 watts per square metre). Importantly, this substantial cooling effect has increased since 1750 by -0.05 ± 0.03 watts per square metre (61 per cent), driven by the anthropogenic amplification of natural halogen emissions, and is projected to change further (18-31 per cent by 2100) depending on climate warming projections and socioeconomic development. We conclude that the indirect radiative effect due to short-lived halogens should now be incorporated into climate models to provide a more realistic natural baseline of Earth's climate system.


Asunto(s)
Atmósfera , Cambio Climático , Modelos Climáticos , Clima , Frío , Halógenos , Atmósfera/análisis , Atmósfera/química , Halógenos/análisis , Hidrocarburos Halogenados , Océanos y Mares , Agua de Mar/análisis , Agua de Mar/química , Cambio Climático/estadística & datos numéricos , Actividades Humanas
2.
Proc Natl Acad Sci U S A ; 121(12): e2315058121, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38466839

RESUMEN

Mercury (Hg) is a contaminant of global concern, and an accurate understanding of its atmospheric fate is needed to assess its risks to humans and ecosystem health. Atmospheric oxidation of Hg is key to the deposition of this toxic metal to the Earth's surface. Short-lived halogens (SLHs) can provide halogen radicals to directly oxidize Hg and perturb the budget of other Hg oxidants (e.g., OH and O3). In addition to known ocean emissions of halogens, recent observational evidence has revealed abundant anthropogenic emissions of SLHs over continental areas. However, the impacts of anthropogenic SLHs emissions on the atmospheric fate of Hg and human exposure to Hg contamination remain unknown. Here, we show that the inclusion of anthropogenic SLHs substantially increased local Hg oxidation and, consequently, deposition in/near Hg continental source regions by up to 20%, thereby decreasing Hg export from source regions to clean environments. Our modeling results indicated that the inclusion of anthropogenic SLHs can lead to higher Hg exposure in/near Hg source regions than estimated in previous assessments, e.g., with increases of 8.7% and 7.5% in China and India, respectively, consequently leading to higher Hg-related human health risks. These results highlight the urgent need for policymakers to reduce local Hg and SLHs emissions. We conclude that the substantial impacts of anthropogenic SLHs emissions should be included in model assessments of the Hg budget and associated health risks at local and global scales.


Asunto(s)
Mercurio , Humanos , Mercurio/toxicidad , Mercurio/análisis , Monitoreo del Ambiente/métodos , Ecosistema , China , India
3.
Proc Natl Acad Sci U S A ; 120(31): e2303974120, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37487065

RESUMEN

Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidation of the potent greenhouse gas methane, causing uncertainty in global methane budgets. We propose a photocatalytic mechanism for chlorine atom production that occurs when Sahara dust mixes with sea spray aerosol. The mechanism is validated by implementation in a global atmospheric model and thereby explaining the episodic, seasonal, and location-dependent 13C depletion in CO in air samples from Barbados [J.E. Mak, G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos. 108 (2003)], which remained unexplained for decades. The production of Cl can also explain the anomaly in the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos. 114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawler et al., Atmos. Chem. Phys. 11, 7617-7628 (2011)]. Our model finds that 3.8 Tg(Cl) y-1 is produced over the North Atlantic, making it the dominant source of chlorine in the region; globally, chlorine production increases by 41%. The shift in the methane sink budget due to the increased role of Cl means that isotope-constrained top-down models fail to allocate 12 Tg y-1 (2% of total methane emissions) to 13C-depleted biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the 13C isotope of atmospheric CH4, thereby partially masking a much greater decline in this isotope, which has implications for the interpretation of the drivers behind the recent increase of methane in the atmosphere.

4.
Proc Natl Acad Sci U S A ; 119(7)2022 02 15.
Artículo en Inglés | MEDLINE | ID: mdl-35131938

RESUMEN

The catalytic depletion of Antarctic stratospheric ozone is linked to anthropogenic emissions of chlorine and bromine. Despite its larger ozone-depleting efficiency, the contribution of ocean-emitted iodine to ozone hole chemistry has not been evaluated, due to the negligible iodine levels previously reported to reach the stratosphere. Based on the recently observed range (0.77 ± 0.1 parts per trillion by volume [pptv]) of stratospheric iodine injection, we use the Whole Atmosphere Community Climate Model to assess the role of iodine in the formation and recent past evolution of the Antarctic ozone hole. Our 1980-2015 simulations indicate that iodine can significantly impact the lower part of the Antarctic ozone hole, contributing, on average, 10% of the lower stratospheric ozone loss during spring (up to 4.2% of the total stratospheric column). We find that the inclusion of iodine advances the beginning and delays the closure stages of the ozone hole by 3 d to 5 d, increasing its area and mass deficit by 11% and 20%, respectively. Despite being present in much smaller amounts, and due to faster gas-phase photochemical reactivation, iodine can dominate (∼73%) the halogen-mediated lower stratospheric ozone loss during summer and early fall, when the heterogeneous reactivation of inorganic chlorine and bromine reservoirs is reduced. The stratospheric ozone destruction caused by 0.77 pptv of iodine over Antarctica is equivalent to that of 3.1 (4.6) pptv of biogenic very short-lived bromocarbons during spring (rest of sunlit period). The relative contribution of iodine to future stratospheric ozone loss is likely to increase as anthropogenic chlorine and bromine emissions decline following the Montreal Protocol.


Asunto(s)
Atmósfera/análisis , Yodo/química , Pérdida de Ozono , Ozono Estratosférico/química , Contaminantes Atmosféricos/química , Regiones Antárticas , Estaciones del Año
5.
Proc Natl Acad Sci U S A ; 118(4)2021 01 26.
Artículo en Inglés | MEDLINE | ID: mdl-33479177

RESUMEN

Reactive iodine plays a key role in determining the oxidation capacity, or cleansing capacity, of the atmosphere in addition to being implicated in the formation of new particles in the marine boundary layer. The postulation that heterogeneous cycling of reactive iodine on aerosols may significantly influence the lifetime of ozone in the troposphere not only remains poorly understood but also heretofore has never been observed or quantified in the field. Here, we report direct ambient observations of hypoiodous acid (HOI) and heterogeneous recycling of interhalogen product species (i.e., iodine monochloride [ICl] and iodine monobromide [IBr]) in a midlatitude coastal environment. Significant levels of ICl and IBr with mean daily maxima of 4.3 and 3.0 parts per trillion by volume (1-min average), respectively, have been observed throughout the campaign. We show that the heterogeneous reaction of HOI on marine aerosol and subsequent production of iodine interhalogens are much faster than previously thought. These results indicate that the fast formation of iodine interhalogens, together with their rapid photolysis, results in more efficient recycling of atomic iodine than currently considered in models. Photolysis of the observed ICl and IBr leads to a 32% increase in the daytime average of atomic iodine production rate, thereby enhancing the average daytime iodine-catalyzed ozone loss rate by 10 to 20%. Our findings provide direct field evidence that the autocatalytic mechanism of iodine release from marine aerosol is important in the atmosphere and can have significant impacts on atmospheric oxidation capacity.

6.
Molecules ; 29(7)2024 Mar 25.
Artículo en Inglés | MEDLINE | ID: mdl-38611742

RESUMEN

Tumor vaccines have been considered a promising therapeutic approach for treating cancer in recent years. With the development of sequencing technologies, tumor vaccines based on neoantigens or genomes specifically expressed in tumor cells, mainly in the form of peptides, nucleic acids, and dendritic cells, are beginning to receive widespread attention. Therefore, in this review, we have introduced different forms of neoantigen vaccines and discussed the development of these vaccines in treating cancer. Furthermore, neoantigen vaccines are influenced by factors such as antigen stability, weak immunogenicity, and biosafety in addition to sequencing technology. Hence, the biological nanomaterials, polymeric nanomaterials, inorganic nanomaterials, etc., used as vaccine carriers are principally summarized here, which may contribute to the design of neoantigen vaccines for improved stability and better efficacy.


Asunto(s)
Vacunas contra el Cáncer , Nanoestructuras , Neoplasias , Ácidos Nucleicos , Humanos , Vacunas contra el Cáncer/uso terapéutico , Medicina de Precisión , Nanoestructuras/uso terapéutico , Neoplasias/terapia
7.
Proc Natl Acad Sci U S A ; 117(9): 4505-4510, 2020 03 03.
Artículo en Inglés | MEDLINE | ID: mdl-32071211

RESUMEN

Dimethyl sulfide (DMS), emitted from the oceans, is the most abundant biological source of sulfur to the marine atmosphere. Atmospheric DMS is oxidized to condensable products that form secondary aerosols that affect Earth's radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report the atmospheric discovery of a previously unquantified DMS oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), identified through global-scale airborne observations that demonstrate it to be a major reservoir of marine sulfur. Observationally constrained model results show that more than 30% of oceanic DMS emitted to the atmosphere forms HPMTF. Coincident particle measurements suggest a strong link between HPMTF concentration and new particle formation and growth. Analyses of these observations show that HPMTF chemistry must be included in atmospheric models to improve representation of key linkages between the biogeochemistry of the ocean, marine aerosol formation and growth, and their combined effects on climate.

8.
Small ; 18(15): e2107452, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35212138

RESUMEN

Although all-inorganic perovskite materials present multiple fascinating optical properties, their poor stability undermines their potential application in the field of multi-color display. Herein, spatially confined CsPbBr3 nanocrystals are in situ crystallized within uniform mesoporous SiO2 nanospheres (MSNs) to regulate their size distribution, passivate their surface defects, shield them from water/oxygen, and more importantly, enhance their thermotolerance. As a result, the remnant PL intensity of the prepared spatially confined perovskite (CsPbBr3 ) nanocrystals by in situ crystallization within uniform mesoporous SiO2 nanospheres (SCP@MSNs) powders can be maintained over 98% of its initial value even after being immersed in harsh conditions (0.1 m HCl or 0.1 m NaOH) for 60 days. Furthermore, the prepared SCP@MSNs-PDMS film demonstrates astonishing thermostability by maintaining almost consistent room temperature PL intensities after continuous heating-cooling cycles between 200 and 25 °C, which would greatly improve its processability during potential industrial manufacturing. The fabricated LCD backlit based on SCP@MSNs covers 124% of NTSC standard and 95.6% of Rec. 2020 standard, indicating its great potential in practical display field.

9.
Geophys Res Lett ; 49(6): e2021GL097567, 2022 Mar 28.
Artículo en Inglés | MEDLINE | ID: mdl-35859565

RESUMEN

Heterogeneous uptake of hypoiodous acid (HOI), the dominant inorganic iodine species in the marine boundary layer (MBL), on sea-salt aerosol (SSA) to form iodine monobromide and iodine monochloride has been adopted in models with assumed efficiency. Recently, field measurements have reported a much faster rate of this recycling process than previously assumed in models. Here, we conduct global model simulations to quantify the range of effects of iodine recycling within the MBL, using Conventional, Updated, and Upper-limit coefficients. When considering the Updated coefficient, iodine recycling significantly enhances gaseous inorganic iodine abundance (∼40%), increases halogen atom production rates (∼40% in I, >100% in Br, and ∼60% in Cl), and reduces oxidant levels (-7% in O3, -2% in OH, and -4% in HO2) compared to the simulation without the process. We appeal for further direct measurements of iodine species, laboratory experiments on the controlling factors, and multiscale simulations of iodine heterogeneous recycling.

10.
Langmuir ; 37(42): 12271-12277, 2021 Oct 26.
Artículo en Inglés | MEDLINE | ID: mdl-34644074

RESUMEN

Pinning of a three-phase contact line at the nanoscale cannot be explained by conventional macroscale theories and thus requires an experimental insight to understand this phenomenon. We performed in-situ transmission electron microscopy observation of the three-phase contact lines of bubbles inside graphene liquid cells to experimentally investigate the causes of nanoscale pinning. In our observations, the three-phase contact line was not affected by the 0.6 nm-thick inhomogeneity of the graphene surface, but thicker metal nanoparticles with diameters of 2-10 nm and nanoflakes caused pinning of the gas-liquid interface. Notably, we found that flake-like objects can cause pinning that prevents the bubble overcome the flake object in a noncontact state, with a 2 nm-thick liquid film between them and the bubble. This phenomenon can be explained by the repulsive force obtained using the Derjaguin, Landau, Verwey, and Overbeek theory. We also observed that the flake temporally prevented the gas-liquid interface moving away from the flake. We discussed the physical mechanism of the attractive force-like phenomenon by considering the nanoconfinement effect of the liquid sandwiched by two graphene sheets and the hydration layer formed near the solid surface.

11.
Environ Sci Technol ; 55(20): 13625-13637, 2021 10 19.
Artículo en Inglés | MEDLINE | ID: mdl-34591460

RESUMEN

Severe and persistent haze events in northern China, characterized by high loading of fine aerosol especially of secondary origin, negatively impact human health and the welfare of ecosystems. However, current knowledge cannot fully explain the formation of this haze pollution. Despite field observations of elevated levels of reactive halogen species (e.g., BrCl, ClNO2, Cl2, HBr) at several sites in China, the influence of halogens (particularly bromine) on haze pollution is largely unknown. Here, for the first time, we compile an emission inventory of anthropogenic bromine and quantify the collective impact of halogens on haze pollution in northern China. We utilize a regional model (WRF-Chem), revised to incorporate updated halogen chemistry and anthropogenic chlorine and bromine emissions and validated by measurements of atmospheric pollutants and halogens, to show that halogens enhance the loading of fine aerosol in northern China (on average by 21%) and especially its secondary components (∼130% for secondary organic aerosol and ∼20% for sulfate, nitrate, and ammonium aerosols). Such a significant increase is attributed to the enhancement of atmospheric oxidants (OH, HO2, O3, NO3, Cl, and Br) by halogen chemistry, with a significant contribution from previously unconsidered bromine. These results show that higher recognition of the impact of anthropogenic halogens shall be given in haze pollution research and air quality regulation.


Asunto(s)
Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , China , Ecosistema , Monitoreo del Ambiente , Halógenos , Humanos , Material Particulado/análisis
12.
Small ; 16(48): e2005639, 2020 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-33169499

RESUMEN

The disordered dendritic growth of Li metal seriously hampers the practical application of lithium metal batteries. Great efforts are devoted to suppress the growth of dendrites, it is still necessary to explore measures of controlling dendritic growth and pave ways for normal cell operation in presence of dendrites. Herein, a modification technique of Li metal anode by a periodic Ni mesh with micrometer-sized grid is proposed for interfacial engineering. Periodic patterned Ni mesh is prepared using a novel laser direct-writing technique combined with selective electrodeposition process. The growth of Li dendrites is regulated under the effect of unique electric field distribution by the introduction of the Ni mesh. It is noteworthy that the controlled lateral growth of dendrites is successfully realized by the internal structure modification instead of any external electric or magnetic field as has been previously reported. The resultant anode exhibits a stable cycling performance with ultralow overpotential of 6-8 mV for over 1000 h at the current density of 0.5 mA cm-2 . It also presents superior electrochemical performance when assembled against LiFePO4 cathode into full cells, with an initial capacity of 133 mA h g-1 and a stable cycling performance over 160 cycles.

13.
Phys Chem Chem Phys ; 22(24): 13629-13636, 2020 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-32519700

RESUMEN

Hydration structures are ubiquitous at solid/liquid interfaces and play a key role in various physicochemical and biological phenomena. Recently, it has been reported that dissolved gas molecules attracted to hydrophobic surfaces form adsorbed gas layers. Although a hydration structure and adsorbed gas layers coexist on the surface, the relationships between them remain unknown. In this study, we investigated a highly ordered pyrolytic graphite/pure water interface with and without adsorbed gas layers using frequency-modulation atomic force microscopy. We penetrated the adsorbed gas layers with the strong load force of the AFM tip and thereby obtained the frequency shift curves inside them. By comparing the curves with those measured on a bare HOPG surface, we found that the adsorbed gas layers were located at regions where the molecular density of water was low and were sandwiched between hydration layers with high water density. Moreover, the distance between adjacent hydration layers was larger than that predicted by simulations and was the same with and without the adsorbed gas layers. We propose that gas molecules on the hydrophobic surface interact with the hydration structure before forming the adsorbed gas layers, and extend the distance between hydration layers.

14.
Atmos Environ (1994) ; 244: 117961, 2020 Oct 29.
Artículo en Inglés | MEDLINE | ID: mdl-33132736

RESUMEN

We implement oceanic dimethylsulfide (DMS) emissions and its atmospheric chemical reactions into the Community Multiscale Air Quality (CMAQv53) model and perform annual simulations without and with DMS chemistry to quantify its impact on tropospheric composition and air quality over the Northern Hemisphere. DMS chemistry enhances both sulfur dioxide (SO2) and sulfate ( S O 4 2 - ) over seawater and coastal areas. It enhances annual mean surface SO2 concentration by +46 pptv and S O 4 2 - by +0.33 µg/m3 and decreases aerosol nitrate concentration by -0.07 µg/m3 over seawater compared to the simulation without DMS chemistry. The changes decrease with altitude and are limited to the lower atmosphere. Impacts of DMS chemistry on S O 4 2 - are largest in the summer and lowest in the fall due to the seasonality of DMS emissions, atmospheric photochemistry and resultant oxidant levels. Hydroxyl and nitrate radical-initiated pathways oxidize 75% of the DMS while halogen-initiated pathways oxidize 25%. DMS chemistry leads to more acidic particles over seawater by decreasing aerosol pH. Increased S O 4 2 - from DMS enhances atmospheric extinction while lower aerosol nitrate reduces the extinction so that the net effect of DMS chemistry on visibility tends to remain unchanged over most of the seawater.

15.
Phys Chem Chem Phys ; 21(4): 1963-1971, 2019 Jan 23.
Artículo en Inglés | MEDLINE | ID: mdl-30633276

RESUMEN

Clay swelling occurs frequently and is closely relevant to a number of engineering and industrial processes, while the underlying mechanisms remain elusive. In this study, K+-bearing clay systems with different charge amounts and charge locations have been simulated by molecular dynamics, showing that swelling is unfavorable for lower charge amounts (1.00 and 1.25 e uc-1) while it relies on charge locations for higher charge amounts (1.50 and 1.75 e uc-1): inhibited when tetrahedrally charged and favored when octahedrally charged. Accordingly, K+ shows dual characteristics and is not always a swelling inhibitor as generally thought. The various influencing factors are inspected and only the hydration effect interprets satisfactorily the swelling behaviors for all K+-bearing clay systems. The critical role of hydration effect during clay swelling is corroborated by the results of residence time, distribution of interlayer water and divergent swelling behaviors from Na+-bearing clay systems. Although water participates in a wide spectrum of physical and chemical processes, hydration is not necessarily among the most important influencing factors. Hydration effect has been evidenced as critical for clay swelling, and the results provide new insights into unraveling the complex swelling processes and resolving the associated engineering and industrial problems.

16.
Environ Sci Technol ; 52(5): 2810-2818, 2018 03 06.
Artículo en Inglés | MEDLINE | ID: mdl-29406712

RESUMEN

Tropospheric ozone pollution has been a major environmental issue, and mitigation of this persistent problem requires a comprehensive understanding of the sensitivity of ozone to its precursors, i.e., nitrogen oxides (NO x) and volatile organic compounds (VOCs). Recent studies have proposed several "new" reactive nitrogen chemical processes, including additional sources of nitrous acid, heterogeneous uptake of dinitrogen pentoxide, and production of nitryl chloride. These processes significantly affect the budgets of radicals and NO x and hence the formation of ozone. In present study, we aim to investigate to what extent these processes alter the relationships between ozone and its precursors. A revised Weather Research and Forecasting model coupled with Chemistry incorporating the "new" nitrogen chemistry was adopted to simulate the ozone sensitivity regime in China in summer. The results showed that nitrogen chemistry changed the ozone sensitivity regime for approximately 40% of the simulated area with human influence, mostly from VOC-sensitive or NO x-sensitive regimes to mixed-sensitive regime. The nitrogen chemistry changed the isopleth plots of the ozone peak values for major cities, suggesting a different strategy for controlling ozone pollution. This study underscores the need to consider unconventional nitrogen chemistry in air quality models used in the design of ozone control strategies.


Asunto(s)
Contaminantes Atmosféricos , Ozono , Compuestos Orgánicos Volátiles , China , Ciudades , Monitoreo del Ambiente , Humanos , Nitrógeno , Óxidos de Nitrógeno
17.
Sci Total Environ ; 945: 174107, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-38908598

RESUMEN

Nitrate (NO3-) has been identified as a key component of particulate matter (PM2.5) in China. However, there is still a lack of understanding regarding its sources and how it forms, especially in the context of high-frequency and long-term data. In this study, NO3- levels were observed on an hourly basis over an almost three-year period at an urban site in the Pearl River Delta (PRD) region, China, from January 2019 to December 2021. The results reveal an average daily NO3- concentration ranging from 0.08 µg m-3 to 61.69 µg m-3, constituting 11.9 ± 12.5 % of PM2.5. This percentage rose to as high as 57 % during pollution episodes, highlighting NO3-'s significant role in pollution formation. The ammonia-rich environment was found to be the most important factor in promoting NO3- formation. Positive Matrix Factorization (PMF) analysis indicates that the primary sources of NO3- in the PRD region were vehicle emissions (43.8 ± 21.2 %) and coal combustion (39.1 ± 21.5 %), with shipping emissions, sea salt, soil dust and industrial emissions + biomass burning following in importance. Regarding source areas, the primary contributor of vehicle emissions was predominantly from the PRD region, whereas the coal combustion, aside from local contributions, also originates from the northern region. From a long-term perspective, NO3- pollution has remained relatively stable since the summer of 2020. Concurrently, coal combustion source has shown a localization trend. These insights derived from the extensive, high-frequency observation presented in this study serve as a valuable reference for devising strategies to control NO3- and PM2.5 in the PRD region and China.

18.
J Hazard Mater ; 468: 133718, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38394891

RESUMEN

Understanding the quantum mechanical mechanisms underlying atomic/ionic interfacial processes and phenomena, particularly their dependence on the electronic orbital rearrangement of atoms/ions in an external electric field, remains a significant challenge. This study investigated the asymmetric response of transition metal (TM) cationic orbitals when subjected to an applied electric field. Quantum mechanical calculations were employed to quantify the newly formed hybrid orbitals and evaluate the corresponding orbital energies of the TM cations. Analysis of the quantitative contribution of asymmetric orbital hybridization to TM-surface interactions showed a significant change in orbital energy and increased effective charges of TM cations at the charged surface. This asymmetric response, induced by a negative external electric field generated from the structural charges of clay minerals (e.g., montmorillonite), repels electrons from the outer-shell orbital. This repulsion consequently increases the electron binding energy of the inner-shell orbitals, leading to new surface reactions, polarization-enhanced induction force, and polarization-induced covalent bonding between the TM cations and the charged surface. Our theoretical predictions regarding TM-clay mineral interactions are consistent with the experimental observations of TM cation adsorption. This finding has significant implications for the adsorptive removal of TM cations from wastewaters and for enhancing the catalytic efficiency of TM-surface catalysts. The unique physical and chemical characteristics exhibited by TMs at charged particle surfaces, resulting from their asymmetric response, can play pivotal roles in environmental and chemical engineering.

19.
Natl Sci Rev ; 11(4): nwae074, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38623452

RESUMEN

Tropospheric reactive bromine is important for atmospheric chemistry, regional air pollution, and global climate. Previous studies have reported measurements of atmospheric reactive bromine species in different environments, and proposed their main sources, e.g. sea-salt aerosol (SSA), oceanic biogenic activity, polar snow/ice, and volcanoes. Typhoons and other strong cyclonic activities (e.g. hurricanes) induce abrupt changes in different earth system processes, causing widespread destructive effects. However, the role of typhoons in regulating reactive bromine abundance and sources remains unexplored. Here, we report field observations of bromine oxide (BrO), a critical indicator of reactive bromine, on the Huaniao Island (HNI) in the East China Sea in July 2018. We observed high levels of BrO below 500 m with a daytime average of 9.7 ± 4.2 pptv and a peak value of ∼26 pptv under the influence of a typhoon. Our field measurements, supported by model simulations, suggest that the typhoon-induced drastic increase in wind speed amplifies the emission of SSA, significantly enhancing the activation of reactive bromine from SSA debromination. We also detected enhanced BrO mixing ratios under high NOx conditions (ppbv level) suggesting a potential pollution-induced mechanism of bromine release from SSA. Such elevated levels of atmospheric bromine noticeably increase ozone destruction by as much as ∼40% across the East China Sea. Considering the high frequency of cyclonic activity in the northern hemisphere, reactive bromine chemistry is expected to play a more important role than previously thought in affecting coastal air quality and atmospheric oxidation capacity. We suggest that models need to consider the hitherto overlooked typhoon- and pollution-mediated increase in reactive bromine levels when assessing the synergic effects of cyclonic activities on the earth system.

20.
Invest Ophthalmol Vis Sci ; 65(3): 12, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38466289

RESUMEN

Purpose: Glaucoma, a leading cause of blindness worldwide, is suspected to exhibit a notable association with psychological disturbances. This study aimed to investigate epidemiological associations and explore shared genetic architecture between glaucoma and mental traits, including depression and anxiety. Methods: Multivariable logistic regression and Cox proportional hazards regression models were employed to investigate longitudinal associations based on UK Biobank. A stepwise approach was used to explore the shared genetic architecture. First, linkage disequilibrium score regression inferred global genetic correlations. Second, MiXeR analysis quantified the number of shared causal variants. Third, specific shared loci were detected through conditional/conjunctional false discovery rate (condFDR/conjFDR) analysis and characterized for biological insights. Finally, two-sample Mendelian randomization (MR) was conducted to investigate bidirectional causal associations. Results: Glaucoma was significantly associated with elevated risks of hospitalized depression (hazard ratio [HR] = 1.54; 95% confidence interval [CI], 1.01-2.34) and anxiety (HR = 2.61; 95% CI, 1.70-4.01) compared to healthy controls. Despite the absence of global genetic correlations, MiXeR analysis revealed 300 variants shared between glaucoma and depression, and 500 variants shared between glaucoma and anxiety. Subsequent condFDR/conjFDR analysis discovered 906 single-nucleotide polymorphisms (SNPs) jointly associated with glaucoma and depression and two associated with glaucoma and anxiety. The MR analysis did not support robust causal associations but indicated the existence of pleiotropic genetic variants influencing both glaucoma and depression. Conclusions: Our study enhances the existing epidemiological evidence and underscores the polygenic overlap between glaucoma and mental traits. This observation suggests a correlation shaped by pleiotropic genetic variants rather than being indicative of direct causal relationships.


Asunto(s)
Depresión , Glaucoma , Humanos , Ansiedad/genética , Ceguera , Depresión/epidemiología , Depresión/genética , Glaucoma/genética , Desequilibrio de Ligamiento
SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA