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Water-insoluble organic carbon (WIOC) constitutes a substantial portion of organic carbon (OC) and contributes significantly to light absorption by brown carbon (BrC), playing pivotal roles in climate forcing. China is a hotspot region with high levels of OC and BrC, but information regarding the sources and light-absorbing properties of WIOC on a national scale remains scarce. Here, we investigated the light-absorbing properties and sources of WIOC in 10 representative urban cities in China. On average, WIOC made up 33.4 ± 7.66 % and 40.5 ± 9.73 % of concentrations and light absorption at 365 nm (Abs 365) of extractable OC (EX-OC), which includes relatively hydrophobic OC (WIOC and humic-like substances, HULIS-C) and hydrophilic OC (non-humic-like substances, non-HULIS-C). The mass absorption efficiency of WIOC at 365 nm (MAE 365) was (1.59 ± 0.55 m2(gC)-1) comparable to that of HULIS (1.54 ± 0.57 m2(gC)-1) but significantly higher than non-HULIS (0.71 ± 0.28 m2(gC)-1), indicating that hydrophobic OC possesses a stronger light-absorbing capacity than hydrophilic OC. Biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of WIOC, with coal combustion sources exhibiting the strongest light-absorbing capacity. Moreover, employing the simple forcing efficiency (SFE 300–700nm) method, we observed that WIOC exhibited the highest SFE 300–700nm (6.57 ± 5.37 Wg-1) among the EX-OC fractions. The radiative forcing of EX-OC was predominantly contributed by hydrophobic OC (WIOC – 39.4 ± 15.5 % and HULIS – 39.5 ± 12.1 %). Considering the aromaticity, sources, and atmospheric processes of different carbonaceous components, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to possess stronger light-absorbing capacity, higher aromatic levels, increased molecular weights, and greater recalcitrance in the atmosphere. Reducing fossil fuel emissions emerges as an effective means of mitigating both gaseous (CO2) and particulate light-absorbing carbonaceous warming components. [ABSTRACT FROM AUTHOR]

Mandatory use of low-sulfur fuel according to global sulfur limit regulation has reduced the emissions of SO2 and PM significantly on ships, while it also leads to very large uncertainty on VOCs emission. Therefore, on-board test of VOCs from 9 typical cargo ships with low-sulfur fuels in China were carried out in this study. Results showed that emission factor of VOCs (EFVOCs) varied largely from 0.09 to 3.01 g kg-1 fuel, with domestic coastal cargo ships (CCSs) had the highest levels and ocean-going vessels (OGVs) the lowest. The switch of fuels from heavy fuel oil (HFO) to diesel increased EFVOCs by 48 % on average, which enhanced both O3 and secondary organic aerosol (SOA) formation potentials, especially for OGVs. Besides, the use of low-sulfur fuels for OGVs also lead to significant increase of naphthalene emission. These indicated the implementation of globally ultra-low-sulfur oil policy in the near future needs to be optimized. Moreover, aromatics were the most important common contributors to O3 and SOA in ship exhausts, which need to be controlled with priority. It was also found that benzene, toluene, and ethylbenzene ratio of 0.5:0.3:0.2 on average could be considered as a diagnostic characteristic to distinguish ship emission from other emission sources. [ABSTRACT FROM AUTHOR]

Water-insoluble carbon (WIOC) constitutes a substantial portion of organic carbon (OC) and contributes significantly to light absorption by brown carbon (BrC), playing pivotal roles in climate forcing and human health. China as hotspots regions with high level of OC and BrC, information regarding the sources and light-absorbing properties of WIOC on national scale remains scarce. Here, we investigated the light-absorbing properties and sources of WIOC in ten representative urban cities across China. On average, WIOC accounted for 33.4 ± 7.66 % and 40.5 ± 9.73 % of the concentrations and light-absorbing efficiency at 365 nm (Abs365) of extractable OC (EX-OC, comprising relatively hydrophobic OC [WIOC and humic-like substances: HULIS-C], and hydrophilic OC [non-humic-like substances: non-HULIS-C]). The mass absorption efficiency of WIOC at 365 nm (MAE365) was (1.59 ± 0.55 m2/gC) comparable to that of HULIS (1.54 ± 0.57 m2/gC) but significantly higher than non-HULIS (0.71 ± 0.28 m2/gC), indicating that hydrophobic OC possesses a stronger light-absorbing capacity than hydrophilic OC. Biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of WIOC, with coal combustion sources exhibited the strongest light-absorbing capacity. Moreover, employing the simple forcing efficiency (SFE300–700nm) method, we observed that WIOC exhibited the highest SFE300–700nm (6.57 ± 5.37 W/g) among the EX-OC fractions. The radiative forcing of EX-OC was predominantly contributed by hydrophobic OC (WIOC: 39.4 ± 15.5 % and HULIS: 39.5 ± 12.1 %). Considering the aromaticity, sources, and atmospheric processes of different carbonaceous components, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to possess stronger light-absorbing capacity, higher aromatic levels, increased molecular weights, and greater recalcitrance in the atmosphere. Reducing fossil fuel emissions emerges as an effective means of mitigating both gaseous (CO2) and particulate light-absorbing carbonaceous warming components. [ABSTRACT FROM AUTHOR]

Humic‐like substances (HULIS) are significant contributor to the light absorption of water‐soluble brown carbon (WSBrC), which contains certain strong light‐absorbing chemical components that are not well understood, impeding the assessment of WSBrC's climate impact. China as the hotspot regions with high loading of WSBrC characterized by high light‐absorbing capacity, here, we investigated the sources and atmospheric processes (δ13C–Δ14C), molecular composition (Fourier transform ion cyclotron resonance mass spectrometry), and light absorption properties (UV spectrophotometry) of HULIS in PM2.5 from 10 Chinese cities. HULIS‐C was major contributor to the light absorption coefficient (70.5 ± 6.6%) of WSBrC at 365 nm, which was more enriched with fossil sources (48.0 ± 9.0% vs. 30.3 ± 13.9%) but depleted in 13C (δ13C: −25.6 ± 0.9‰ vs. −22.4 ± 1.0‰) relative to non‐HULIS‐C. This suggests that the fossil components in HULIS are more recalcitrant to oxidative aging and exhibit higher light‐absorbing capacity, while the non‐fossil organic carbon is more likely to be oxidatively bleached into small, colorless, and highly polar molecules (i.e., non‐HULIS). Aromatic components are the major strong light‐absorbing fossil components in HULIS, dominantly originating from coal combustion (>77%). Non‐negative matrix factorization model showed that aromatic molecules from coal combustion have higher molecular weight and lower oxidation levels than biomass burning, potentially making them to be photo‐recalcitrant compounds. Our finding that coal combustion‐derived BrC maybe more persistent in the atmosphere and has greater long‐term impact on climate than BrC derived from biomass burning is an important consideration in climate models and mitigation policies. Plain Language Summary: Both the loading and light‐absorbing capacity of water‐soluble brown carbon (WSBrC) are high in China, but little is known about sources and atmospheric processes of strong light‐absorbing components in WSBrC. Humic‐like substances (HULIS) account for a significant fraction of light absorption by WSBrC, which may contain strong light‐absorbing components. Through dual carbon isotopic analysis, we discovered that HULIS‐C from 10 Chinese cities had relatively higher fossil sources contribution but lower δ13C values compared to non‐HULIS‐C. This indicates that the fossil components in HULIS not only possess a higher light‐absorbing capacity but are also more resistant to oxidative aging than non‐fossil components. The higher light‐absorbing capacity and resilience of fossil components can be attributed to the enrichment of aromatic compounds derived from coal combustion. Using the non‐negative matrix factorization model, we found that coal combustion tends to generate aromatic compounds with higher molecular weight and lower oxidation‐to‐carbon (O/C: 0.31 ± 0.03 vs. 0.50 ± 0.07) ratios than biomass burning. This characteristic may contribute to the recalcitrant property of coal combustion‐derived HULIS. Our findings highlight that coal combustion‐derived BrC may persists longer in the atmosphere and has a greater long‐term impact on climate than that derived from biomass burning. [ABSTRACT FROM AUTHOR]

The Bohai Sea (BS) region, an area of China that is severely polluted with atmospheric polycyclic aromatic hydrocarbons (PAHs), has received wide attention in recent decades. To characterize the variations of the concentrations and sources of PAHs from June 2014 to May 2019, 15 PAH congeners (Σ15PAHs) were measured in atmospheric samples (N = 228) collected at 12 sites around the BS, and the health risk and direct medical costs associated with lung cancer caused by exposure to PAHs were also estimated. The annual daily average concentration of Σ15PAHs was 56.78 ± 4.75 ngm-3 , which was dominated by low molecular weight PAHs (LMW-PAHs) containing three rings (58.7 ± 7.8 %). During the 5-year sampling period, the atmospheric Σ15PAHs concentration reduced by 17.5 % for the whole BS region, with an especially large drop of 51.7 % observed in the tightly controlled area of Tianjin (TJ), which was mainly due to a decrease in the concentration of high molecular weight PAHs (HMW-PAHs) containing five or six rings. Generally, the concentration of Σ15PAHs was highest in winter and lowest in summer, which can mainly be attributed to the change in LMW-PAH concentration. Based on the positive matrix factorization (PMF) model, PAHs in the BS region were mainly ascribed to coal combustion and biomass burning. The PAH contributions of coal combustion and motor vehicles showed different trends for the BS region (PAHs from coal combustion rose by 7.2 % and PAHs from motor vehicles fell by 22.4 %) and for TJ (PAHs from coal combustion fell by 12.6 % and PAHs from motor vehicles rose by 6.9 %). The incidence of lung cancer (ILCR) caused by exposure to atmospheric PAHs decreased by 74.1 % and 91.6 % from 2014 to 2018 in the BS region and in TJ, respectively. This was mainly due to the decrease in the concentration of highly toxic HMW-PAHs and was reflected in USD 10.7 million of savings in direct medical costs of lung cancer caused by exposure to PAHs, which represent a decrease of 46.1 % compared to the corresponding costs before air pollution prevention and control was implemented around the BS. There was an even higher reduction in medical costs of 54.5 % in TJ. Hence, this study proves that implementing pollution prevention and control not only effectively reduced the concentration of pollutants and the risks caused by them, but it also significantly reduced the medical costs of diseases caused by the corresponding exposure. [ABSTRACT FROM AUTHOR]

The nitrogen stable isotope composition (δ15 N) of nitrogen oxides (NO x) is a powerful indicator of source apportionment of atmospheric NO x ; however, δ15 N–NO x values emitted from ships have not been reported, affecting the accuracy of source partitioning of atmospheric NO x in coastal zones with a lot of vessel activity. In addition, δ15 N–NO x values from ship emissions could also be important for source apportionment of atmospheric nitrogen deposition in remote ocean regions. This study systemically analysed the δ15 N–NO x variability and main influencing factors of ship emissions. The results showed that δ15 N–NO x values from ships, which were calculated by weighting the emission values from the main engine and auxiliary engine of the vessel, ranged from - 35.8 ‰ to 2.04 ‰ with a mean ± standard deviation of - 18.5 ± 10.9 ‰. The δ15 N–NO x values increased monotonically with the ongoing tightening of emission regulations, presenting a significantly negative logarithmic relationship with NO x concentrations (p<0.01). The selective catalytic reduction (SCR) system was the most important factor affecting changes in δ15 N–NO x values, followed by the ship category, fuel types, and operation states of ships. Based on the relationship between δ15 N–NO x values and emission regulations observed in this investigation, a mass-weighted model to compute accurate assessments over time was developed, and the temporal variation in δ15 N–NO x values from ship emissions in the international merchant fleet was evaluated. These simulated δ15 N–NO x values can be used to select suitable δ15 N–NO x values for a more accurate assessment, including the contribution of ship-emitted exhaust to atmospheric NO x and its influence on atmospheric nitrate (NO 3-) air quality and nitrogen deposition studies. [ABSTRACT FROM AUTHOR]