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Brown carbon (BrC) contributes significantly to aerosol light absorption and thus can affect the Earth's radiation balance and atmospheric photochemical processes. In this study, we examined the light absorption properties and molecular compositions of water-soluble (WS-BrC) and water-insoluble (WI-BrC) BrC in PM2.5 collected from a rural site in the Guanzhong Basin – a highly polluted region in northwest China. Both WS-BrC and WI-BrC showed elevated light absorption coefficients (Abs) in winter (4–7 times those in summer) mainly attributed to enhanced emissions from residential biomass burning (BB) for heating of homes. While the average mass absorption coefficients (MACs) at 365 nm (MAC365) of WS-BrC were similar between daytime and nighttime in summer (0.99±0.17 and 1.01±0.18 m2 g−1, respectively), the average MAC365 of WI-BrC was more than a factor of 2 higher during daytime (2.45±1.14 m2 g−1) than at night (1.18±0.36 m2 g−1). This difference was partly attributed to enhanced photochemical formation of WI-BrC species, such as oxygenated polycyclic aromatic hydrocarbons (OPAHs). In contrast, the MACs of WS-BrC and WI-BrC were generally similar in winter and both showed few diel differences. The Abs of wintertime WS-BrC correlated strongly with relative humidity, sulfate and NO2, suggesting that aqueous-phase reaction is an important pathway for secondary BrC formation during the winter season in northwest China. Nitrophenols on average contributed 2.44±1.78 % of the Abs of WS-BrC in winter but only 0.12±0.03 % in summer due to faster photodegradation reactions. WS-BrC and WI-BrC were estimated to account for 0.83±0.23 % and 0.53±0.33 %, respectively, of the total down-welling solar radiation in the ultraviolet (UV) range in summer, and 1.67±0.72 % and 2.07±1.24 %, respectively, in winter. The total absorption by BrC in the UV region was about 55 %–79 % relative to the elemental carbon (EC) absorption.

As a renewable and environment-friendly technology for seawater desalination and wastewater purification, solar energy triggered steam generation is attractive to address the long-standing global water scarcity issues. However, practical utilization of solar energy for steam generation is severely restricted by the complex synthesis, low energy conversion efficiency, insufficient solar spectrum absorption and water extraction capability of state-of-the-art technologies. Here, for the first time, we report a facile strategy to realize hydrogen bond induced self-assembly of a polydopamine (PDA)@MXene microsphere photothermal layer for synergistically achieving wide-spectrum and highly efficient solar absorption capability (≈ 96% in a wide solar spectrum range of 250–1,500 nm wavelength). Moreover, such a system renders fast water transport and vapor escaping due to the intrinsically hydrophilic nature of both MXene and PDA, as well as the interspacing between core-shell microspheres. The solar-to-vapor conversion efficiencies under the solar illumination of 1 sun and 4 sun are as high as 85.2% and 93.6%, respectively. Besides, the PDA@MXene photothermal layer renders the system durable mechanical properties, allowing producing clean water from seawater with the salt rejection rate beyond 99%. Furthermore, stable light absorption performance can be achieved and well maintained due to the formation of ternary TiO2/C/MXene complex caused by oxidative degradation of MXene. Therefore, this work proposes an attractive MXene-assisted strategy for fabricating high performance photothermal composites for advanced solar-driven seawater desalination applications.

The Himalayas and Tibetan Plateau (the HTP), referred to as “the third pole” with an excessive warming rate, exerts strong impacts on the global environment. As one of warming contributors, atmospheric brown carbon (BrC) remains limited scientific understanding in the HTP due to a scarcity of observations. In this study, we present a study of the light‐absorbing properties of methanol‐soluble brown carbon (MeS‐BrC) and water‐soluble brown carbon (WS‐BrC) during 2018–2021. Highly spatiotemporal variations of BrC light absorptions were observed. In the HTP marginal area, elevated BrC absorption coefficients at 365 nm (babs,365) and levoglucosan concentrations were obtained, and MeS‐BrC exhibits approximately 1.3–1.8 times higher absorption compared to WS‐BrC. We determined that BrC light absorptions was largely attributed to biomass burning (29%–35%). BrC can act as a potent warming agent in the HTP marginal area, with high direct solar absorption (25%–47% relative to black carbon). Plain Language Summary Atmospheric brown carbon (BrC) remains low scientific understanding in the HTP due to a scarcity of observations. Here, we present a plateau‐scale study of the light‐absorbing properties of methanol‐soluble brown carbon (MeS‐BrC) and water‐soluble brown carbon (WS‐BrC) during the period of 2018–2021. This study highlights the contribution of BrC to the HTP warming. Higher BrC light absorption was observed in the HTP marginal area compared with the central HTP. Enhanced radiative absorption effect of WS‐BrC was obtained in the HTP, with an annual average of ∼25% compared with BC in Qinghai Lake and Ngari, and as high as 46.5% in Purang. The results confirmed the importance of BrC from biomass burning in contributing to light‐absorbing aerosols in this region. Key Points Brown carbon (BrC) can be a strong warming agent in the marginal Himalayas and Tibetan Plateau Highly spatiotemporal variations of plateau‐scale BrC were observed BrC light absorptions was largely attributed to biomass burning

Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1; emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.

Brown carbon (BrC) in China is of great interest to the regional and global climate due to its strong absorption of sunlight. However, the contribution of BrC to total carbonaceous aerosol light absorption and its direct radiative effects (DRE) in China remains largely uncertain. To better assess its climate impact in China, we develop an explicit BrC scheme and implement it in a global climate model, which includes optical parameters of primary BrC derived from local measurements, secondary BrC absorption, and a photobleaching parameterization of BrC. By comparing with multi‐type observational data, we find that with the implementation of this scheme, the model captures the seasonal variations of BrC light absorption well in China. The model estimates that BrC contributes 19% and 12% to the total light absorption of carbonaceous aerosol in China in winter and summer, resulting in 0.110 and 0.205 W m−2 of DRE, respectively. Plain Language Summary While the existing research on the direct radiative effects (DRE) of brown carbon (BrC) predominantly focuses on biomass‐burning sources, little attention has been given to BrC originating from anthropogenic sources. Coal combustion and residential fuels used for cooking and heating release many brown carbon aerosols in China. Source of BrC in China is different from that in Europe and North America. Therefore, studying the light‐absorbing properties and climate effects of BrC in China is of great scientific significance. Here, we introduce local optical parameters of primary BrC based on observations in China, secondary BrC absorption, and chemical bleaching of BrC in a global climate model (GCM). We find that the model can simulate the strong seasonal variations of BrC absorption observed in China. With the help of the model and multi‐type measurement data, we estimate the contribution of BrC to the total carbonaceous aerosol absorption and the DRE of BrC in China in different seasons. This study is the first attempt to introduce an explicit BrC scheme in a GCM to estimate the DRE of BrC in China. Key Points An explicit brown carbon (BrC) scheme is introduced in a climate model together with observations to constrain light absorption of BrC BrC contributes 19% and 12% of total carbonaceous aerosol absorption in China in winter and summer, respectively Simulated direct radiative effects due to BrC absorption over China are 0.110 and 0.205 W m2 in the winter and summer seasons

Atmospheric black carbon (BC), the strongest absorber of visible solar radiation in the atmosphere, manifests across a wide spectrum of morphologies and compositional heterogeneity. Phenomenologically, the distribution of BC among diverse particles of varied composition gives rise to enhancement of its light absorption capabilities by over twofold in comparison to that of nascent or unmixed homogeneous BC. This situation has challenged the modeling community to consider the full complexity and diversity of BC on a per-particle basis for accurate estimation of its light absorption. The conventionally adopted core–shell approximation, although computationally inexpensive, is inadequate not only in estimating but also capturing absorption trends for ambient BC. Here we develop a unified framework that encompasses the complex diversity in BC morphology and composition using a single metric, the phase shift parameter (ρBC), which quantifies how much phase shift the incoming light waves encounter across a particle compared to that in its absence. We systematically investigate variations in ρBC across the multi-space distribution of BC morphology, mixing state, mass, and composition as reported by field and laboratory observations. We find that ρBC>1 leads to decreased absorption by BC, which explains the weaker absorption enhancements observed in certain regional BC compared to laboratory results of similar mixing state. We formulate universal scaling laws centered on ρBC and provide physics-based insights regarding core–shell approximation overestimating BC light absorption. We conclude by packaging our framework in an open-source Python application to facilitate community-level use in future BC-related research. The package has two main functionalities. The first functionality is for forward problems, wherein experimentally measured BC mixing state and assumed BC morphology are input, and the aerosol absorption properties are output. The second functionality is for inverse problems, wherein experimentally measured BC mixing state and absorption are input, and the morphology of BC is returned. Further, if absorption is measured at multiple wavelengths, the package facilitates the estimation of the imaginary refractive index of coating materials by combining the forward and inverse procedures. Our framework thus provides a computationally inexpensive source for calculation of absorption by BC and can be used to constrain light absorption throughout the atmospheric lifetime of BC.

Nitro-aromatic compounds (NACs), as important contributors to the light absorption by brown carbon, have been widely observed in various ambient atmospheres; however, their formation in the urban atmosphere was little studied. In this work, we report an intensive field study of NACs in summer 2016 at an urban Beijing site, characterized by both high-NOx and anthropogenic VOC dominated conditions. We investigated the factors that influence NAC formation (e.g., NO2, VOC precursors, RH and photolysis) through quantification of eight NACs, along with major components in fine particulate matter, selected volatile organic compounds, and gases. The average total concentration of the quantified NACs was 6.63 ng m-3, higher than those reported in other summertime studies (0.14–6.44 ng m-3). 4-Nitrophenol (4NP, 32.4 %) and 4-nitrocatechol (4NC, 28.5 %) were the top two most abundant NACs, followed by methyl-nitrocatechol (MNC), methyl-nitrophenol (MNP), and dimethyl-nitrophenol (DMNP). The oxidation of toluene and benzene in the presence of NOx was found to be a more dominant source of NACs than primary biomass burning emissions. The NO2 concentration level was found to be an important factor influencing the secondary formation of NACs. A transition from low- to high-NOx regimes coincided with a shift from organic- to inorganic-dominated oxidation products. The transition thresholds were NO2∼20 ppb for daytime andNO2∼25 ppb for nighttime conditions. Under low-NOx conditions, NACs increased with NO2, while the NO3- concentrations and (NO3-)/NACs ratios were lower, implying organic-dominated products. Under high-NOx conditions, NAC concentrations did not further increase with NO2, while theNO3- concentrations and (NO3-)/NACs ratios showed increasing trends, signaling a shift from organic- to inorganic-dominated products. Nighttime enhancements were observed for 3M4NC and 4M5NC, while daytime enhancements were noted for 4NP, 2M4NP, and DMNP, indicating different formation pathways for these two groups of NACs. Our analysis suggested that the aqueous-phase oxidation was likely the major formation pathway of 4M5NC and 3M5NC, while photo-oxidation of toluene and benzene in the presence of NO2 could be more important for the formation of nitrophenol and its derivatives. Using the (3M4NC+4M5NC) / 4NP ratios as an indicator of the relative contribution of aqueous-phase and gas-phase oxidation pathways to NAC formation, we observed that the relative contribution of aqueous-phase pathways increased at elevated ambient RH and remained constant at RH > 30 %. We also found that the concentrations of VOC precursors (e.g., toluene and benzene) and aerosol surface area acted as important factors in promoting NAC formation, and photolysis as an important loss pathway for nitrophenols.

Scientific knowledge about light absorption by aerosols is extremely limited at the eastern slope of the Tibetan Plateau (ESTP). We conducted the first aerosol field experiment at six sites (Chengdu, Sanbacun, Wenchuan, Lixian, Maerkang, Hongyuan) along the ESTP, ranging in elevation from 500 to 3500 m. The fraction of light absorption by brown carbon (BrC) to total carbon increases from 20 % to 50 % with altitude, and the mass absorption efficiency (MAE) of BrC over the Tibetan Plateau (TP) is 2–3 times higher than that inside the Sichuan Basin (SCB), especially in winter. In contrast, the MAE of elemental carbon (EC) in winter decreases with altitude. The contrasting variation of EC and BrC MAE with altitude is mainly attributed to source differences between the TP and SCB. Emissions from the more urban sources (motor vehicles, industries, etc.) inside the SCB fail to be transported to the TP due to the stable air in winter inside the basin, which is also favourable for aerosol ageing to enhance absorption efficiency. The radiative forcing of BrC relative to EC varies from 0.10 to 0.42 as altitude increases with the higher organic carbon (OC) to EC ratio over the TP than SCB. Thus, the reason for the enhanced relative BrC to EC radiative forcing from polluted SCB to pristine TP is that the BrC concentration decreases more slowly than the EC concentration with altitude. This study contributes to the understanding of the difference in light absorption by EC and BrC with altitude, from polluted lower-altitude basins to the pristine TP, and provides a data set for regional climate model validation.

Atmospheric brown carbon (BrC) makes a substantial contribution to aerosol light absorption and thus global radiative forcing. Although BrC may change the lifetime of the clouds and ultimately affect precipitation, little is known regarding the optical properties and formation of BrC in the clouds. In the present study, the light-absorption properties of cloud droplet residual (cloud RES) were measured by coupled a ground-based counterflow virtual impactor (GCVI) and an aethalometer (AE-33), in addition to the cloud interstitial (cloud INT) and ambient (cloud-free) particles by PM2.5 inlet-AE-33 at Mt. Tianjing (1690 m a.s.l.), a remote mountain site in southern China, from November to December 2020. Meanwhile, the light-absorption and fluorescence properties of water-soluble organic carbon (WSOC) in the collected cloud water and PM2.5 samples were also obtained, associated with the concentration of water-soluble ions. The mean light-absorption coefficient (Abs370) of the cloud RES, cloud INT, and cloud-free particles were 0.25 ± 0.15, 1.16 ± 1.14, and 1.47 ± 1.23 Mm−1, respectively. The Abs365 of WSOC was 0.11 ± 0.08 Mm−1 in cloud water and 0.40 ± 0.31 Mm−1 in PM2.5, and the corresponding mass absorption efficiency (MAE365) was 0.17 ± 0.07 and 0.31 ± 0.21 m2 g−1, respectively. A comparison of the light-absorption coefficient between BrC in cloud RES and cloud INT particles, and WSOC in cloud water and PM2.5 indicates a considerable contribution (48 %–75 %) of water-insoluble BrC to total BrC light absorption. Secondary BrC estimated by minimum R squared (MRS) method dominated the total BrC in cloud RES (67 %–85 %), rather than in the cloud-free (11 %–16 %) and cloud INT (9 %–23 %) particles. It may indicate the formation of secondary BrC during cloud processing. Supporting evidence includes the enhanced WSOC and dominant contribution of the secondary formation and biomass burning factor (>80 %) to Abs365 in cloud water provided by positive matrix factorization (PMF) analysis. In addition, we showed that the light absorption of BrC in cloud water was closely related to humic-like substances and tyrosine-like and/or protein-like substances (r>0.63, p<0.01), whereas only humic-like substances for PM2.5, as identified by excitation-emission matrix fluorescence spectroscopy.

Secondary organic aerosols (SOAs) formed by oxidation of typical precursors largely emitted by biomass burning, such as polycyclic aromatic hydrocarbons (PAHs) and furans, are still poorly characterized. We evaluated and compared the formation yields, effective density (ρeff), absorption Ångström exponent (α), and mass absorption coefficient (MAC) of laboratory-generated SOAs from three furan compounds and four PAHs. SOAs were generated in an oxidation flow reactor under day- (OH radicals) or nighttime (NO3 radicals) conditions. The ρeff, formation yields, α, and MAC of the generated SOAs varied depending on the precursor and oxidant considered. The ρeff of SOAs formed with OH and NO3 tended to increase with particle size before reaching a “plateau”, highlighting potential differences in SOA chemical composition and/or morphology, according to the particle size. Three times lower SOA formation yields were obtained with NO3 compared with OH. The yields of PAH SOAs (18 %–76 %) were five to six times higher than those obtained for furans (3 %–12 %). While furan SOAs showed low or negligible light absorption properties, PAH SOAs had a significant impact in the UV–visible region, implying a significant contribution to atmospheric brown carbon. No increase in the MAC values was observed from OH to NO3 oxidation processes, probably due to a low formation of nitrogen-containing chromophores with NO3 only (without NOx). The results obtained demonstrated that PAHs are significant SOA precursors emitted by biomass burning, through both, day- and nighttime processes, and have a substantial impact on the aerosol light absorption properties.