Atmospheric heterogeneous reaction of chlorobenzene on mineral α-Fe2O3 particulates: a chamber experiment study

doi:10.1007/s11783-023-1734-9

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (11) : 134 https://doi.org/10.1007/s11783-023-1734-9

RESEARCH ARTICLE

Atmospheric heterogeneous reaction of chlorobenzene on mineral α-Fe₂O₃ particulates: a chamber experiment study

Meiling Chen^1,², Mengjie Yin³, Yuetan Su¹, Ruizhe Li¹, Kezhou Liu³, Zhongbiao Wu^1,⁴, Xiaole Weng^1,^2,⁴(

)

¹. Key Laboratory of Environment Remediation and Ecological Health (Ministry of Education), College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
². ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China
³. School of Automation (School of Artificial Intelligence), Hangzhou Dianzi University, Hangzhou 310018, China
⁴. Zhejiang Provincial Engineering Research Centre of Industrial Boiler & Furnace Flue Gas Pollution Control, Hangzhou 311200, China

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Abstract

● Photochemical conversion of chlorobenzene (CB) on α-Fe₂O₃ was evaluated.

● CB can be considerably degraded by α-Fe₂O₃ under light irradiation.

● Photochemical conversion of CB is markedly suppressed by adding SO₂ or NO₂.

● CB can be ultimately converted into PCDD/Fs under dark state or light irradiation.

● Photochemical conversion complements an overlooked source of natural PCDD/Fs.

Despite the large emission of chlorinated volatile organic compounds (CVOCs) into the atmosphere, the ultimate fate of these compounds remains largely unknown. Herein, we explore the photochemical conversion of an important class of CVOCs, namely chlorobenzene (CB), on mineral α-Fe₂O₃ particulates under atmospheric relevant conditions. A series of chamber reactions composed of the CB with/without SO₂ or NO₂ are performed, followed by in situ diffuse reflectance infrared Fourier transform spectroscopy measurements and density functional theory calculations. We show that CB can be considerably degraded by α-Fe₂O₃ under light irradiation, whereas the reaction is markedly suppressed by adding SO₂ or NO₂ owing to their competitive adsorption and surface acidification. In particular, we discover that CB can be ultimately converted into polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) under dark state or light irradiation, suggesting a possible origin of atmospheric PCDD/Fs from this overlooked photochemical source.

Keywords Photochemical conversion Chlorobenzene α-Fe₂O₃ PCDD/Fs Mineral particulate

Corresponding Author(s): Xiaole Weng

About author:

^* These authors contributed equally to this work.

Issue Date: 15 November 2023

Cite this article:

Meiling Chen,Mengjie Yin,Yuetan Su, et al. Atmospheric heterogeneous reaction of chlorobenzene on mineral α-Fe₂O₃ particulates: a chamber experiment study[J]. Front. Environ. Sci. Eng., 2023, 17(11): 134.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1734-9
https://academic.hep.com.cn/fese/EN/Y2023/V17/I11/134

Fig.1 Decay rates of CB in the absence and presence of α-Fe₂O₃ particulates in the chamber experiments. (a) Schematic diagram of the chamber setup; (b) CB + O₂ reaction; (c) CB + SO₂ + O₂ reaction; (d) CB + NO₂ + O₂ reaction. Reaction conditions: [CB] = 200 ppm, [SO₂] = [NO₂] = 50 ppm, air balance, 30 °C and xenon light irradiation (λ = 320–780 nm). Error bars represent standard deviation.

Fig.2 Results of the reaction byproduct analysis. (a) Distribution of gas-phase byproducts, (b) volatile, and (c) semi-volatile organic byproducts on the α-Fe₂O₃ surface after 7 h of reaction. (d) The result of CPs after 35 h of reaction based on SIM in a GC/MS system. Reaction conditions: [CB] = 200 ppm, [SO₂] = [NO₂] = 50 ppm, air balance, 30 °C and xenon light irradiation (λ = 320–780 nm).

Fig.3 In situ DRIFT spectra of α-Fe₂O₃ as a function of time with a flow of CB and SO₂ or NO₂ in the absence and presence of light. Reaction conditions: [CB] = 200 ppm, [SO₂] = [NO₂] = 50 ppm, [O₂] = 20 vol %, 30 °C and xenon light irradiation (λ = 320–780 nm).

Fig.4 The atmospheric heterogeneous photochemical reaction mechanism of CB on the surface of α-Fe₂O₃.

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