Advanced modeling of the absorption enhancement of black carbon particles in chamber experiments by considering the morphology and coating thickness

doi:10.1007/s11783-024-1876-4

2024, Vol. 18

Issue (9) : 116 https://doi.org/10.1007/s11783-024-1876-4

Advanced modeling of the absorption enhancement of black carbon particles in chamber experiments by considering the morphology and coating thickness

Xiaodong Wei^1,^2,^3,⁴, Jianlin Hu¹(

), Chao Liu², Xiaodong Xie¹, Junjie Yin¹, Song Guo⁵, Min Hu⁵, Jianfei Peng⁶, Huijun Wang^2,³(

)

¹. Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, Nanjing 210044, China
². Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Key Laboratory of Meteorological Disaster (Ministry of Education), Nanjing University of Information Science and Technology, Nanjing 210044, China
³. Nansen−Zhu International Research Centre, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
⁴. East China Air Traffic Management Bureau CAAC, Shanghai 200335, China
⁵. State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control (IJRC) (Ministry of Education), College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
⁶. Tianjin Key Laboratory of Urban Transport Emission Research & State Environmental Protection Key Laboratory of Urban Ambient Air Particulate Matter Pollution Prevention and Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300071, China

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Abstract

● CS structure overestimates ρ _eff by nearly six times at externally mixed states.

● FA method reproduces the evolution of BCc morphology.

● MSTM can reproduce a more realistic evolution of optical properties.

● A two-stage calibration of E _abs as the function of coating fractions is developed.

Measurements studies have shown that the absorption of radiation by black carbon (BC) increases as the particles age. However, there are significant discrepancies between the measured and modeled absorption enhancement (E_abs), largely due to the simplifications used in modeling the mixing states and shape diversities. We took advantage of chamber experiments on BC aging and developed an efficient method to resolve the particle shape based on the relationship between the coating fraction (∆D_ve/D_ve,0) and fractal dimension (D_f), which can also reflect the variations of D_f during the whole BC aging process. BC with externally and partly mixed states (0 ≤ ∆D_ve/D_ve,0 ≤ 0.5) can be considered to be uniformly distributed with the D_f values of 1.8–2.1, whereas the D_f values are constrained in the range 2.2–2.8 for fully mixed states (∆D_ve/D_ve,0 > 0.5). The morphological parameters (i.e., the effective density and the dynamic shape factor) were compared with the measured values to verify the simulated morphology. The simulated mean deviations of morphological parameters were smaller than 8% for the method resolving the particle shape. By applying a realistic shape and refractive index, the mass absorption cross for fully mixed states can be improved by 11% compared with a simplified core–shell model. Based on our understanding of the influence of D_f and ∆D_ve/D_ve,0 on E_abs, we propose a two-stage calibration equation to correct the E_abs values estimated by the core–shell model, which reduces the simulation error in the Mie calculation by 6%–14%.

Keywords Black carbon Mixing states Fractal dimension Dynamic shape factor Absorption enhancement

Corresponding Author(s): Jianlin Hu,Huijun Wang

Issue Date: 05 July 2024

Cite this article:

Xiaodong Wei,Jianlin Hu,Chao Liu, et al. Advanced modeling of the absorption enhancement of black carbon particles in chamber experiments by considering the morphology and coating thickness[J]. Front. Environ. Sci. Eng., 2024, 18(9): 116.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-024-1876-4
https://academic.hep.com.cn/fese/EN/Y2024/V18/I9/116

Fig.1 The morphological evolution of BCc showing the measured

χ

and

ρ e f f

values as a function of the coating fraction with initial mobility diameters of about (a) 100 nm, (b) 150 nm, and (c) 220 nm. The blue and red shading show the modeled values of F_ns as a function of the coating fraction.

Fig.2 Quantitative evolution of the shape parameters for partially mixed states showing

χ

and ρ_eff as a function of the coating fraction for the FA model (solid lines), the CS model (dashed lines) and the observations (OBS) (symbols). The shading shows the model errors considering the ranges of D_f for experiments conducted with initial BC mobility diameters of about (a) and (b) 100 nm, (c) and (d) 150 nm, (e) and (f) 220 nm.

Fig.3 Quantitative evolution of the shape parameters for the fully mixed states showing the ρ_eff (a) and

χ

(b) values with initial mobility diameters of about 100, 150, and 220 nm, respectively. The square symbols show the mean values, the top and bottom of the boxes show the upper and lower quartiles and the boundary lines show the minimum and maximum values.

Method	Parameter	Externally mixed	Partly coated	Fully coated
Observations	ρ _eff	0.27±0.04–0.46±0.03	0.35±0.07–1.17±0.05	1.30±0.05
Observations	$χ$	2.22±0.08–2.70±0.23	1.14±0.03–2.44±0.20	1.05±0.04
FA model	ρ _eff	0.34±0.12–0.44±0.15	0.35±0.13–1.25±0.42	1.29±0.04
	$χ$	2.29±0.44–2.48±0.46	1.14±0.22–2.44±0.45	1.06±0.03
	Geometry
CS model	ρ _eff	1.77	1.47–1.76	1.41±0.03
	$χ$	1.00	1.00	1.00
	Geometry

Tab.1 Observational and numerical ρ_eff (g/cm³) and

χ

values for the three mixing states when considering three initial mobilities of about 100, 150, and 220 nm

Fig.4 The MAC simulated by the Mie and MSTM models as a function of the real and imaginary parts of the RI at wavelengths of (a, b) 405 nm and (d, e) 532 nm. (c, f) show the biases between the Mie and MSTM calculations.

Fig.5 The MAC at wavelengths of 405 nm (a) and 532 nm (b) modeled as a function of the imaginary part of RI. The hexagonal and spherical symbols represent the values from the Mie and MSTM models and the color bar is the relative deviation between the simulations and observations.

Tab.2 Comparison of retrieved RI based on observations from the chamber method. The corresponding MAC values and relative errors are also listed

Fig.6 Comparisons of MSTM model (solid line), the Mie model (dashed line) and the measured MAC with changes in the coating fraction at wavelengths of (a) 405 nm and (b) 532 nm. The error bars and shading region represent the SD.

Fig.7 Discrepancy in E_abs between the Mie and MSTM models with a change in the fractal dimension and coating fraction at wavelengths of (a) 405 nm and (b) 532 nm.

Fig.8 The two-stage variation in ?E_abs as a function of the coating fraction showing the mean (dashed lines) and error (shading) values for ?E_abs with a change in the coating fraction at wavelengths of (a) 405 nm and (b) 532 nm.

Fig.9 Comparisons of the revised Mie model (solid line), the Mie model (dashed line) and the QUALITY MAC with changes in the coating fraction at wavelengths of (a) 405 nm and (b) 532 nm. The error bars and shading region represent the SD.

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