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Great progress has been made in organic solar cells (OSCs) in recent years, especially after the report of the highly efficient small-molecule electron acceptor Y6. However, the relatively low open circuit voltage (VOC) and unbalanced charge mobilities remain two issues that need to be resolved for further improvement in the performance of OSCs. Herein, a wide-band-gap amorphous acceptor IO-4Cl, which possessed a shallower lowest unoccupied molecular orbital (LUMO) energy level than Y6, was introduced into the PM6:Y6 binary system to construct a ternary device. The mechanism study revealed that the introduced IO-4Cl was alloyed with Y6 to prevent the overaggregation of Y6 and offer dual channels for effective hole transportation, resulting in balanced hole and electron mobilities. Taking these advantages, an enhanced VOC of 0.894 V and an improved fill factor of 75.58% were achieved in the optimized PM6:Y6:IO-4Cl-based ternary device, yielding a promising power conversion efficiency (PCE) of 17.49%, which surpassed the 16.72% efficiency of the PM6:Y6 binary device. This work provides an alternative solution to balance the charge mobilities of PM6:Y6-based devices by incorporating an amorphous high-performance LUMO A-D-A small molecule as the third compound.
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With the rapid development of small-molecule electron acceptors, polymer electron donors are becoming more important than ever in organic photovoltaics, and there is still room for the currently available high-performance polymer donors. To further develop polymer donors with finely tunable structures to achieve better photovoltaic performances, random ternary copolymerization is a useful technique. Herein, by incorporating a new electron-withdrawing segment 2,3-bis(3-octyloxyphenyl)dithieno[3,2-f:2',3'-h]quinoxaline derivative (C12T-TQ) to PM6, a series of terpolymers were synthesized. It is worth noting that the introduction of the C12T-TQ unit can deepen the highest occupied molecular orbital energy levels of the resultant polymers. In addition, the polymer Z6 with a 10% C12T-TQ ratio possesses the highest film absorption coefficient (9.86 × 104 cm-1) among the four polymers. When blended with Y6, it exhibited superior miscibility and mutual crystallinity enhancement between Z6 and Y6, suppressed recombination, better exciton separation and charge collection characteristics, and faster hole transfer in the D-A interface. Consequently, the device of Z6:Y6 successfully achieved enhanced photovoltaic parameters and yielded an efficiency of 17.01%, higher than the 16.18% of the PM6:Y6 device, demonstrating the effectiveness of the meta-octyloxy-phenyl-modified dithieno[3,2-f:2',3'-h]quinoxaline moiety to build promising terpolymer donors for high-performance organic solar cells.
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Atmospheric pollution has detrimental effects on human health and ecosystems. The southern region of the Himalayas, undergoing rapid urbanization and intense human activities, faces poor air quality marked by high aerosol loadings. In this study, we conducted a two-year PM10 sampling in the suburban area (Godavari) of Kathmandu, a representative metropolis situated in the southern part of the central Himalayas. The trace elements were measured to depict aerosol-bound element loadings, seasonality, and potential sources. The mean concentrations of trace elements varied considerably, ranging from 0.27 ± 0.19 ng m-3 for Tl to 1252.78 ng m-3 for Zn. The average concentration of Co and Ni was 1.2 and 22.4 times higher, respectively, than those in Lhasa city in Tibet in the northern Himalayas. The concentration of Pb was 38 times lower than that in Lahore, Pakistan, and 9 times lower than urban sites in India. For the seasonality, the trace element concentrations displayed remarkable variation, with higher concentrations during the non-monsoon seasons and lower concentrations during the monsoon season. This trend was primarily influenced by anthropogenic activities such as low-grade fuel combustion in vehicles, coal combustion in brick kilns, and biomass burning, along with seasonal rainfall that induced aerosol washout. The enrichment factors (EFs) analysis revealed that Cd, Zn, Sb, Ni, Cu, Cr, and Pb had higher EFs, indicating their significant contributions from anthropogenic sources. In contrast, elements like Tl, Co, V, Cs, U, Ba, Th, and Sr, characterized by lower EFs, were mainly associated with natural sources. The Pb isotopic ratio profiles exhibited the Pb in PM10 are derived major contribution from legacy lead. Biomass burning contributed to the Pb source in winter. These findings provide policymakers with valuable insights to develop guidelines and strategies aimed at improving air quality and mitigating the impact of aerosol pollution on human health in the Himalayan region.
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Contaminantes Atmosféricos , Oligoelementos , Humanos , Contaminantes Atmosféricos/análisis , Oligoelementos/análisis , Monitoreo del Ambiente , Ecosistema , Himalayas , Plomo/análisis , Aerosoles/análisisRESUMEN
Atmospheric phosphorus is a vital nutrient for ecosystems whose sources and fate are still debated in the fragile Himalayan region, hindering our comprehension of its local ecological impact. This study provides novel insights into atmospheric phosphorus based on the study of total suspended particulate matter at the Qomolangma station. Contrary to the prevailing assumptions, we show that biomass burning (BB), not mineral dust, dominates total dissolved phosphorus (TDP, bioavailable) deposition in this arid region, especially during spring. While total phosphorus is mainly derived from dust (77% annually), TDP is largely affected by the transport of regional biomass-burning plumes from South Asia. During BB pollution episodes, TDP causing springtime TDP fluxes alone accounts for 43% of the annual budget. This suggests that BB outweighs dust in supplying bioavailable phosphorus, a critical nutrient, required to sustain Himalayas' ecological functions. Overall, this first-hand field evidence refines the regional and global phosphorus budget by demonstrating that BB emission, while still unrecognized, is a significant source of P, even in the remote mountains of the Himalayas. It also reveals the heterogeneity of atmospheric phosphorus deposition in that region, which will help predict changes in the impacted ecosystems as the deposition patterns vary.
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Contaminantes Atmosféricos , Biomasa , Contaminantes Atmosféricos/análisis , Fósforo , Ecosistema , Himalayas , Polvo/análisis , Material Particulado/análisis , Minerales , Proteínas de Unión al ADN , Monitoreo del Ambiente , Aerosoles/análisisRESUMEN
Himalayas and Tibetan Plateau (HTP) is important for global biodiversity and regional sustainable development. While numerous studies have revealed that the ecosystem in this unique and pristine region is changing, their exact causes are still poorly understood. Here, we present a year-round (23 March 2017 to 19 March 2018) ground- and satellite-based atmospheric observation at the Qomolangma monitoring station (QOMS, 4276 m a.s.l.). Based on a comprehensive chemical and stable isotope (15N) analysis of nitrogen compounds and satellite observations, we provide unequivocal evidence that wildfire emissions in South Asia can come across the Himalayas and threaten the HTP's ecosystem. Such wildfire episodes, mostly occurring in spring (March-April), not only substantially enhanced the aerosol nitrogen concentration but also altered its composition (i.e., rendering it more bioavailable). We estimated a nitrogen deposition flux at QOMS of â¼10 kg N ha-1 yr-1, which is approximately twice the lower value of the critical load range reported for the Alpine ecosystem. Such adverse impact is particularly concerning, given the anticipated increase of wildfire activities in the future under climate change.
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Contaminantes Atmosféricos , Incendios Forestales , Ecosistema , Tibet , Nitrógeno/análisis , Nitrógeno/química , Aerosoles/análisis , Monitoreo del Ambiente , Contaminantes Atmosféricos/análisisRESUMEN
Aerosols affect the radiative forcing of the global climate and cloud properties. Organic aerosols are among the most important, yet least understood, components of the sensitive Tibetan Plateau atmosphere. Here, the concentration of and the seasonal and diurnal variations in biomass burning and biogenic aerosols, and their contribution to organic aerosols in the inland Tibetan Plateau were investigated using molecular tracers. Biomass burning tracers including levoglucosan and its isomers, and aromatic acids showed higher concentrations during winter than in summer. Molecular tracers of primary and secondary biogenic organic aerosols were more abundant during summer than those in winter. Meteorological conditions were the main factors influencing diurnal variations in most organic molecular tracers during both seasons. According to the tracer-based method, we found that biogenic secondary organic aerosols (38.5 %) and fungal spores (14.4 %) were the two dominant contributors to organic aerosols during summer, whereas biomass burning (15.4 %) was an important aerosol source during winter at remote continental background site. Results from the positive matrix factor source apportionment also demonstrate the importance of biomass burning and biogenic aerosols in the inland Tibetan Plateau. During winter, the long-range transport of biomass burning from South Asia contributes to organic aerosols. In contrast, the precursors, biogenic secondary organic aerosols, and fungal spores from local emissions/long-range transport are the major sources of organic aerosols during summer. Further investigation is required to distinguish between local emissions and the long-range transport of organic aerosols. In-depth insights into the organic aerosols in the Tibetan Plateau are expected to reduce the uncertainties when evaluating aerosol effects on the climate system in the Tibetan Plateau.
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Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Tibet , Ácidos , Estaciones del Año , Aerosoles/análisis , Monitoreo del Ambiente/métodos , Material Particulado/análisis , BiomasaRESUMEN
Owing to the impact of the western development of China, there have been signs of air pollution over the Qinghai-Tibet Plateau in recent years. However, monitoring data on atmospheric volatile organic compounds (VOCs) are lacking in plateau areas. Here, VOCs concentrations in urban and background areas in North China and the Qinghai-Tibet Plateau were observed from 2012 to 2014 and 2020 to 2022, respectively. Compared to 2012-2014, the concentration of VOCs increased to 2.5 times in urban areas on the Qinghai-Tibet Plateau, which was equivalent to that in North China. Oil, gas, and solvent evaporation caused by a low atmospheric pressure is the primary factor for the increase in VOCs in plateau areas, and weak VOCs degradation is the secondary factor. Hence, we put forward the VOCs control strategies in plateau areas and point out the defects in the current research.
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Airborne bacteria are an influential component of the Earth's microbiomes, but their community structure and biogeographic distribution patterns have yet to be understood. We analyzed the bacterial communities of 370 air particulate samples collected from 63 sites around the world and constructed an airborne bacterial reference catalog with more than 27 million nonredundant 16S ribosomal RNA (rRNA) gene sequences. We present their biogeographic pattern and decipher the interlacing of the microbiome co-occurrence network with surface environments of the Earth. While the total abundance of global airborne bacteria in the troposphere (1.72 × 1024 cells) is 1 to 3 orders of magnitude lower than that of other habitats, the number of bacterial taxa (i.e., richness) in the atmosphere (4.71 × 108 to 3.08 × 109) is comparable to that in the hydrosphere, and its maximum occurs in midlatitude regions, as is also observed in other ecosystems. The airborne bacterial community harbors a unique set of dominant taxa (24 species); however, its structure appears to be more easily perturbed, due to the more prominent role of stochastic processes in shaping community assembly. This is corroborated by the major contribution of surface microbiomes to airborne bacteria (averaging 46.3%), while atmospheric conditions such as meteorological factors and air quality also play a role. Particularly in urban areas, human impacts weaken the relative importance of plant sources of airborne bacteria and elevate the occurrence of potential pathogens from anthropogenic sources. These findings serve as a key reference for predicting planetary microbiome responses and the health impacts of inhalable microbiomes with future changes in the environment.
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Microbiología del Aire , Microbiota , Efectos Antropogénicos , Bacterias/genética , Humanos , Microbiota/genética , ARN Ribosómico 16S/genéticaRESUMEN
An empirical model to estimate global solar radiation was developed at Qomolangma Station using observed solar radiation and meteorological parameters. The predicted hourly global solar radiation agrees well with observations at the ground in 2008-2011. This model was used to calculate global solar radiation at the ground and its loss in the atmosphere due to absorbing and scattering substances in 2007-2020. A sensitivity analysis shows that the responses of global solar radiation to changes in water vapor and scattering factors (expressed as water-vapor pressure and the attenuation factor, AF, respectively) are nonlinear, and global solar radiation is more sensitive to changes in scattering than to changes in absorption. Further applying this empirical model, the albedos at the top of the atmosphere (TOA) and the surface in 2007-2020 were computed and are in line with satellite-based retrievals. During 2007-2020, the mean estimated annual global solar radiation increased by 0.22% per year, which was associated with a decrease in AF of 1.46% and an increase in water-vapor pressure of 0.37% per year. The annual mean air temperature increased by about 0.16 °C over the 14 years. Annual mean losses of solar radiation caused by absorbing and scattering substances and total loss were 2.55, 0.64, and 3.19 MJ m-2, respectively. The annual average absorbing loss was much larger than the scattering loss; their contributions to the total loss were 77.23% and 22.77%, indicating that absorbing substances play significant roles. The annual absorbing loss increased by 0.42% per year, and scattering and total losses decreased by 2.00% and 0.14% per year, respectively. The estimated and satellite-derived annual albedos increased at the TOA and decreased at the surface. This study shows that solar radiation and its interactions with atmospheric absorbing and scattering substances have played key but different roles in regional climate and climate change at the three poles.
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Atmósfera , Energía Solar , Cambio Climático , Vapor , TemperaturaRESUMEN
Redox-active quinone and nonquinone moieties represent the electron exchange capacity (EEC) of natural organic matter (NOM), playing an important role in the electron transfer link of microbes and transformation of contaminants/metal minerals. However, the corresponding transformation of quinone/phenol and their respective influence on the EECs during reduction and reoxidation remain poorly characterized. Besides, it is still controversial whether nonquinones donate or accept electrons. Herein, we demonstrated that reoxidation of NOM after reduction can form new phenolic/quinone moieties, thus increasing the EEC. The assessment for the EEC, including the electron-donating capacity (EDC) and electron-accepting capacity (EAC), of nonquinones reflects the contribution of sulfur-containing moieties with considerable EDCs and EACs. In contrast, nitrogen-containing moieties donate negligible electrons even at Eh = +0.73 V. The contributions of both thiol and amine moieties to the EEC are greatly affected by adjacent functional groups. Meanwhile, aldehydes/ketones did not display an EAC during the electron transfer process of NOM. Furthermore, substantially increased EDC at Eh from +0.61 to +0.73 V could not be fully explained using thiol and phenolic moieties, suggesting the contribution of unknown moieties with high oxidation potential. The overall findings suggest that the roles of new quinones/phenol (derived from the addition of oxygen to condensed aromatic/lignin-like components) during redox dynamic cycling and thiol species should be considered in assessing the electron transfer processes of NOM.
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Electrones , Quinonas , Benzoquinonas , Oxidación-Reducción , Fenoles , Compuestos de SulfhidriloRESUMEN
As an important component of carbonaceous aerosols (CA), organic carbon (OC) exerts a strong, yet insufficiently constrained perturbation of the climate. In this study, we reported sources of OC based on its natural abundance radiocarbon (14C) fingerprinting in aerosols and water-insoluble organic carbon (WIOC) in snowpits across the Tibetan Plateau (TP) - one of the remote regions in the world and a freshwater reservoir for billions of people. Overall, the proportions from 14C-based non-fossil fuel contribution (fnon-fossil) for OC in aerosols was 74 ± 10%, while for WIOC in snowpits was 81 ± 10%, both of which were significantly higher than that of elemental carbon (EC). These indicated sources of OC (WIOC) and EC were different at remote TP. Spatially, high fnon-fossil of WIOC of snowpit samples appeared at the inner part of the TP, indicating the important contribution of local non-fossil sources. Therefore, local non-fossil sources rather than long-range transportation OC dominants its total amount of the TP. In addition, the contribution of local non-fossil sourced WIOC increased during the monsoon period because heavy precipitation removed a high ratio of long-range transportation WIOC. The results of this study showed that not only OC and EC but also their different fuel sources should be treated separately in models to investigate their sources and atmospheric transportation.
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Contaminantes Atmosféricos , Carbono , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Atmósfera , Carbono/análisis , Monitoreo del Ambiente/métodos , Humanos , Cubierta de Hielo , Material Particulado/análisis , Estaciones del Año , Tibet , AguaRESUMEN
Deposition of atmospheric mercury (Hg) is the most important Hg source on the high-altitude Himalayas and Tibetan Plateau. Herein, total gaseous Hg (TGM) at an urban and a forest site on the Tibetan Plateau was collected respectively from May 2017 to October 2018, and isotopic compositions were measured to clarify the influences of landforms and monsoons on the transboundary transport of atmospheric Hg to the Tibetan Plateau. The transboundary transported anthropogenic emissions mainly originated over Indo-Gangetic Plain and carried over the Himalayas by convective storms and mid-tropospheric circulation, contributing over 50% to the TGM at the Lhasa urban site, based on the binary mixing model of isotopes. In contrast, during the transport of TGM from South Asia with low altitude, the uptake by evergreen forest in Yarlung Zangbo Grand Canyon largely decreased the TGM level and shifted isotopic compositions in TGM at the Nyingchi forest site, which are located at the high-altitude end of the canyon. Our results provided direct evidence from Hg isotopes to reveal the distinct patterns of transboundary transport to the Tibetan Plateau shaped by landforms and climates, which is critical to fully understand the biogeochemical cycling of Hg in the high-altitude regions.
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Mercurio , Monitoreo del Ambiente/métodos , Isótopos , Mercurio/análisis , Isótopos de Mercurio/análisis , TibetRESUMEN
Formation pathways and sources of atmosphere nitrate (NO3-) have attracted much attention as NO3- had detrimental effects on Earth's ecosystem and climate change. Here, we measured nitrogen (δ15N-NO3-) and oxygen (δ18O-NO3- and Δ17O-NO3-) isotope compositions in nitrate aerosols at the Qomolangma station (QOMS) over the Himalayan-Tibetan Plateau (HTP) to quantify the formation mechanisms and emission sources of nitrate at the background site. At QOMS, the enhanced NO3- concentrations were observed in the springtime. The average δ15N-NO3-, δ18O-NO3-, and Δ17O-NO3- values were 0.4 ± 4.9, 64.7 ± 11.5 and 27.6 ± 6.9, respectively. Seasonal variations of isotope ratios at QOMS can be explained by the different emissions and formation pathways to nitrate. The average fractions of NO2 + OH and N2O5 + H2O to nitrate production were estimated to be 43 and 52%, respectively, when the NO3 + hydrocarbon (HC)/dimethyl sulfide (DMS) (NO3 + HC/DMS) pathway was assumed to be 5%. Using stable isotope analysis in the R (SIAR) model, the relative contributions of biomass burning (BB), biogenic soil emission, traffic, and coal combustion to nitrate were estimated to be 28, 25, 24, and 23%, respectively, on yearly basis. By FLEXible PARTicle (FLEXPART) dispersion model, we highlighted that NOx from BB emission over South Asia that had undergone N2O5 + H2O processes enhanced the nitrate concentrations in the springtime over the HTP region.
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Nitratos , Nitrógeno , Aerosoles , China , Ecosistema , Monitoreo del Ambiente , Nitratos/análisis , Nitrógeno/análisis , Isótopos de Nitrógeno/análisis , Isótopos de Oxígeno/análisis , TibetRESUMEN
Atmospheric aerosols play a crucial role in climate change, especially in the Himalayas and Tibetan Plateau. Here, we present the seasonal and diurnal characteristics of aerosol vertical profiles measured using a Mie lidar, along with surface black carbon (BC) measurements, at Mt. Qomolangma (QOMS), in the central Himalayas, in 2018-2019. Lidar-retrieved profiles of aerosols showed a distinct seasonal pattern of aerosol loading (aerosol extinction coefficient, AEC), with a maximum in the pre-monsoon (19.8 ± 22.7 Mm-1 of AEC) and minimum in the summer monsoon (7.0 ± 11.2 Mm-1 of AEC) seasons. The diurnal variation characteristics of AEC and BC were quite different in the non-monsoon seasons with enriched aerosols being maintained from 00:00 to 10:00 in the pre-monsoon season. The major aerosol types at QOMS were identified as background, pollution, and dust aerosols, especially during the pre-monsoon season. The occurrence of pollution events influenced the vertical distribution, seasonal/diurnal patterns, and types of aerosols. Source contribution of BC based on the weather research and forecasting chemical model showed that approximately 64.2% ± 17.0% of BC at the QOMS originated from India and Nepal in South Asia during the non-monsoon seasons, whereas approximately 47.7% was from local emission sources in monsoon season. In particular, the high abundance of BC at the QOMS in the pre-monsoon season was attributed to biomass burning, whereas anthropogenic emissions were the likely sources during the other seasons. The maximum aerosol concentration appeared in the near-surface layer (approximately 4.3 km ASL), and high concentrations of transported aerosols were mainly found at 4.98, 4.58, 4.74, and 4.88 km ASL in the pre-monsoon, monsoon, post-monsoon, and winter seasons, respectively. The investigation of the vertical profiles of aerosols at the QOMS can help verify the representation of aerosols in the air quality model and satellite products and regulate the anthropogenic disturbance over the Tibetan Plateau.
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Contaminantes Atmosféricos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente , India , Estaciones del Año , Hollín/análisisRESUMEN
Fluorescence spectroscopy is a commonly used technique to analyze dissolved organic matter in aquatic environments. Given the high sensitivity and non-destructive analysis, fluorescence has recently been used to study water-soluble organic carbon (WSOC) in atmospheric aerosols, which have substantial abundance, various sources and play an important role in climate change. Yet, current research on WSOC characterization is rather sparse and limited to a few isolated sites, making it challenging to draw fundamental and mechanistic conclusions. Here we presented a review of the fluorescence properties of atmospheric WSOC reported in various field and laboratory studies, to discuss the current advances and limitations of fluorescence applications. We highlighted that photochemical reactions and relevant aging processes have profound impacts on fluorescence properties of atmospheric WSOC, which were previously unnoticed for organic matter in aquatic environments. Furthermore, we discussed the differences in sources and chemical compositions of fluorescent components between the atmosphere and hydrosphere. We concluded that the commonly used fluorescence characteristics derived from aquatic environments may not be applicable as references for atmospheric WSOC. We emphasized that there is a need for more systematic studies on the fluorescence properties of atmospheric WSOC and to establish a more robust reference and dataset for fluorescence studies in atmosphere based on extensive source-specific experiments.
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Contaminantes Atmosféricos , Carbono , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Carbono/análisis , Monitoreo del Ambiente , Fluorescencia , Material Particulado/análisis , AguaRESUMEN
Strengthening the research of riverine mercury (Hg) export is of great significance for understanding the regional and global Hg cycle, especially for the data lacking trans-Himalayan rivers. In this study, three systematic sampling campaigns were conducted in the Koshi River Basin (KRB) during the post-monsoon, pre-monsoon and monsoon seasons. Hg speciation and distribution of river water were analyzed among the different seasons for a total of 88 water samples. The total Hg (THg) concentration of surface water in the KRB ranged from 0.64 to 32.96 ng·L-1 with an average of 5.83 ± 6.19 ng·L-1 and decreased in the order of post-monsoon (8.79 ± 7.32 ng·L-1) > monsoon (6.68 ± 6.12 ng·L-1) > pre-monsoon (2.18 ± 1.29 ng·L-1). Particulate Hg (PHg) accounted for 63% of THg on average and had a positive correlation with THg among all the three sampling seasons, indicating that the differences in PHg concentration were likely one of the main factors leading to the seasonal and spatial variations in THg in the KRB surface water. The annual Hg exports and fluxes were estimated to be 339.04 kg and 3.88 µg·m-2·yr-1, respectively. Furthermore, Hg export from the KRB had significant seasonal variation and decreased in the order of monsoon (259.47 kg) > post-monsoon (61.18 kg) > winter (9.31 kg) > pre-monsoon (9.08 kg), and this pattern was mainly related to seasonal changes in river runoff. The annual Hg export is projected to increase in the future, especially in the post-monsoon season. Therefore, more attention should be paid to river runoff observations and riverine Hg research for water resources management in the Himalaya.
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Recently, benefiting from the merits of small-molecule acceptors (NFAs), polymer solar cells (PSCs) have achieved tremendous advances. From the perspective of the structural characteristics of the π-conjugated acceptor-donor-acceptor (A-D-A) type of organic molecules, the backbone's planarity and the terminal groups and their substituents have strong influences on the performances of the constructed NFAs. Through enlarging the dihedral angle of the conjugated main chain of NFAs, a certain degree of enhancement of photovoltaic parameters has been achieved. To further probe the influences of ending groups on the performances of nonplanar NFAs, we synthesized two new NFAs i-cc23 and i-cc34 with isomerized thiophene-fused ending groups and a twisted π-conjugated main chain. Compared to i-cc23 containing the 2-(6-oxo-5,6-dihydro-4H-cyclopenta[b]thiophen-4-ylidene)malononitrile ending group, the acceptor i-cc34 containing 2-(6-oxo-5,6-dihydro-4H-cyclopenta[c]thiophen-4-ylidene)malononitrile has a relatively higher molar extinction coefficient, bathochromic-shifted absorption spectrum, and deepened energy levels. When mixed with PBDB-T in solar cells, the i-cc23-based device achieved an excellent open-circuit voltage (VOC) of 1.10 V and a moderate power conversion efficiency of 7.34%. Although the VOC of the i-cc34-related device was decreased to 0.96 V, the short-circuit current density and fill factor were improved, giving rise to an enhanced efficiency of 9.51%. Apart from the distinct photovoltaic performances, the two isomer-based devices exhibit a high radiative efficiency of 8 × 10-4, leading to a very small nonradiative loss of 0.19 V. Our results emphasize the importance of the isomerized thiophene-fused ending groups on the performances of nonplanar NFA-based PSCs.
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Recently, main-chain twisted small molecules are attractive as electron-acceptors in polymer solar cells (PSCs) for their upshifted molecular energy levels, enhanced extinction coefficients, and better charge extraction properties along with longer carrier lifetimes and lower recombination rates relative to their planar analogues, which are conducive to the power conversion efficiency (PCE) promotion of PSCs. To further probe the "structure-performance" correlation of main-chain twisted acceptors, in particular the monofluorine-substituted sites on the performances of the resultant acceptors, two new main-chain twisted small molecules were synthesized, in which a fluorine atom was introduced at different sites on the end-capping group 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (INCN). Although fine structural modification was adopted, quite different performances were obtained for the two acceptors. Compared to the 3-fluorinated analogue (i-IEICO-F3), a mixture of 4-fluorinated and 5-fluorinated isomers (i-IEICO-2F) exhibited a higher dipole moment, enlarged molar extinction coefficient with a bathochromic-shifted absorption region, suppressed charge recombinations with balanced charge mobilities, and slightly enhanced crystallinity. In combination with a fluorobenzotriazole-based medium-band gap polymer (J52), a high efficiency of 12.86% was resultantly achieved in an i-IEICO-2F-based device, which is superior to the result (7.65%) of the i-IEICO-F3 device, revealing the importance of monofluorinated positions on the performances of main-chain twisted non-fullerene acceptors.
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Brown carbon (BrC) has been proposed as an important driving factor in climate change due to its light absorption properties. However, our understanding of BrC's chemical and optical properties are inadequate, particularly at remote regions. This study conducts a comprehensive investigation of BrC aerosols in summer (Aug. 2013) and winter (Jan. 2014) at Southeast Tibetan Plateau, which is ecologically fragile and sensitive to global warming. The concentrations of methanol-soluble BrC (MeS-BrC) are approximately twice of water-soluble BrC (WS-BrC), demonstrating the environmental importance of water-insoluble BrC are previously underestimated with only WS-BrC considered. The mass absorption efficiency of WS-BrC (0.27-0.86â¯m2â¯g-1) is lower than those in heavily polluted South Asia, indicating a distinct contrast between the two sides of Himalayas. Fluorescence reveals that the absorption of BrC is mainly attributed to humic-like and protein-like substances, which broaden the current knowledge of BrC's chromophores. Combining organic tracer, satellite MODIS data and air-mass backward trajectory analysis, this study finds BrC is mainly derived from bioaerosols and secondary formation in summer, while long-range transport of biomass burning emissions in winter. Our study provides new insights into the optical and chemical properties of BrC, which may have implications for environmental effect and sources of organic aerosols.