Quantifying anthropogenic emission of iron in marine aerosol in the Northwest Pacific with shipborne online measurements.

Anthropogenic emissions are recognized as significant contributors to atmospheric soluble iron (Fe) in recent years, which may affect marine primary productivity, especially in Fe-limited areas. However, the contribution of different emission sources to Fe in marine aerosol has been primarily estimated by modeling approaches. Quantifying anthropogenic Fe based on field measurements remains a great challenge. In this study, online multi-element measurements and Positive Matrix Factorization (PMF) were combined for the first time to quantify sources of atmospheric Fe and soluble Fe in the Northwest Pacific during a cruise in spring 2015. Fe concentration in 624 atmospheric PM2.5 samples measured online was 74.58 ± 90.87 ng/m3. The PMF results showed anthropogenic activities, including industrial coal combustion, biomass burning, and maritime transport, were important in this region, contributing 31.4 % of atmospheric Fe on average. In addition, anthropogenic Fe concentration resolved by PMF was comparable to the simulation results of the CMAQ (Community Multiscale Air Quality) and GEOS-Chem (Goddard Earth Observing System-Chemical transport) models, with better correlation to CMAQ (r = 0.76) than GEOS-Chem (r = 0.26). This study developed a new method to estimate atmospheric soluble Fe, which integrates Fe source apportionment results and Fe solubility from different sources. Soluble Fe concentration was estimated as 3.93 ± 5.14 ng/m3, of which 87.0 % was attributed to anthropogenic emissions. Notably, ship emission alone contributed 27.5 % of soluble Fe, though its contribution to total Fe was only 2.2 %. Finally, the total deposition fluxes of atmospheric Fe (37.11 ± 38.43 µg/m2/day) and soluble Fe (1.85 ± 2.13 µg/m2/day) were estimated. This study developed a new methodology for quantifying contribution of anthropogenic emissions to Fe in marine aerosol, which could greatly help the assessment of impacts of human activities on marine environment.

Dynamics of protein condensates in weak-binding regime.

Weak complementary interactions between proteins and nucleic acids are the main driving forces of intracellular liquid-liquid phase separation. The sticker-spacer model has emerged as a unifying principle for understanding the phase behavior of these multivalent molecules. It remains elusive how specific interactions mediated by stickers contribute to the rheological properties of the liquid condensates. Previous studies have revealed that for strong binding strength ɛ_{b}, the bulk diffusivity D depends on the effective bond lifetime τ, viz., D∝τ^{-1}. Consequently, equal concentrations of the complementary stickers induce a slow down in the dynamics of the condensates D∝e^{-1.5ɛ_{b}}. However, for weak-binding strength, it is expected that the resulting condensates are dynamic, loose network liquids rather than kinetically arrested, compact clusters. We develop a mean-field theory using the thermodynamics of the associative polymers and perform molecular-dynamics simulations based on the sticker-spacer model to study the controlling factors in the structure and dynamics of such condensates in the weak-binding regime. Through scaling analysis, we delineate how the free sticker fraction W_{f} and the bulk diffusivity D decrease with increasing binding energy and find that the internal dynamics of such network liquids are controlled by the free sticker fraction D∝W_{f}∝e^{-0.5ɛ_{b}} rather than the effective bond lifetime. Referred to as the free-sticker-dominated diffusivity, the microscopic slowdown due to a gradual loss of the free stickers affects the viscosity of the condensates as well, with the scaling of the zero-shear viscosity η∝e^{0.5ɛ_{b}}. Therefore, the way of controlling the structure, diffusivity, and viscosity of the condensates through the binding energy can be tested experimentally.

Intercomparison of equivalent black carbon (eBC) and elemental carbon (EC) concentrations with three-year continuous measurement in Beijing, China.

Due to the lack of black carbon (BC) measurement data in some cases, elemental carbon (EC) is often used as a surrogate of BC, with a simple assumption that they are interchangeable. Such assumption will inevitably lead to uncertainties in radiative forcing estimation and health impact assessment. In order to quantitatively and systematically evaluate the relationship between BC and EC as well as factors responsible for their difference, 3-year collocated equivalent BC (eBC) and EC measurements with 1-h resolution were performed in Beijing, China continuously from 2016 to 2019. EBC concentration was measured by the multi-wavelength aethalometer (AE-33) based on optical analysis, while EC concentration was determined by semi-continuous OC/EC analyzer with thermal-optical method. The results showed that around 90% of eBC concentration was higher than that of EC, with average difference between eBC and EC as 1.21 µg m-3 (accounting for 33% of average eBC in Beijing). EBC and EC concentrations exhibited strong correlation (r = 0.90) during the whole study period, but the slopes (or eBC/EC ratio) and correlation coefficients varied across seasons (spring: 1.67 and 0.94; summer: 0.91 and 0.65; fall: 1.15 and 0.88; winter: 1.09 and 0.91, respectively). Based on the information from shell/core ratios by Single Particle Soot Photometer (SP2), source apportionment results by positive matrix factorization model, and chemical composition of PM2.5, the differences between eBC and EC concentrations were found to be primarily related to BC aging process and secondary components as evidenced by strong positive correlation with secondary species (e.g., secondary organic carbon and nitrate). This study provided seasonal specific conversion factors of eBC and EC in Beijing and helpful reference for other areas, which will contribute new knowledge of carbonaceous aerosol and reduce uncertainty in assessing future climate change and health studies of BC.