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经臭氧老化的黑碳对二氧化硫的非均相氧化作用及其二硫苏糖醇氧化潜力

Heterogeneous oxidation of SO2 by O3-aged black carbon and its dithiothreitol oxidative potential.

作者信息

Xu Weiwei, Li Qian, Shang Jing, Liu Jia, Feng Xiang, Zhu Tong

机构信息

State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China.

State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China; POTEN Environment Group Co., Ltd., Beijing 100082, China.

出版信息

J Environ Sci (China). 2015 Oct 1;36:56-62. doi: 10.1016/j.jes.2015.02.014. Epub 2015 Jun 26.

Abstract

Ozone (O3) is an important atmospheric oxidant. Black carbon (BC) particles released into the atmosphere undergo an aging process via O3 oxidation. O3-aged BC particles may change their uptake ability toward trace reducing gases such as SO2 in the atmosphere, leading to different environmental and health effects. In this paper, the heterogeneous reaction process between O3-aged BC and SO2 was explored via in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Combined with ion chromatography (IC), DRIFTS was used to qualitatively and quantitatively analyze the sulfate product. The results showed that O3-aged BC had stronger SO2 oxidation ability than fresh BC, and the reactive species/sites generated on the surface had an important role in the oxidation of SO2. Relative humidity or 254nm UV (ultraviolet) light illumination enhanced the oxidation uptake of SO2 on O3-aged BC. The oxidation potentials of the BC particles were detected via dithiothreitol (DTT) assay. The DTT activity over BC was decreased in the process of SO2 reduction, with the consumption of oxidative active sites.

摘要

臭氧(O₃)是一种重要的大气氧化剂。排放到大气中的黑碳(BC)颗粒会通过O₃氧化经历老化过程。经O₃老化的BC颗粒可能会改变其对大气中痕量还原气体(如SO₂)的吸收能力,从而导致不同的环境和健康影响。本文通过原位漫反射红外傅里叶变换光谱(DRIFTS)研究了经O₃老化的BC与SO₂之间的非均相反应过程。结合离子色谱(IC),利用DRIFTS对硫酸盐产物进行定性和定量分析。结果表明,经O₃老化的BC比新鲜BC具有更强的SO₂氧化能力,且表面生成的活性物种/位点在SO₂氧化中起重要作用。相对湿度或254nm紫外(UV)光照增强了经O₃老化的BC对SO₂的氧化吸收。通过二硫苏糖醇(DTT)测定法检测了BC颗粒的氧化电位。在SO₂还原过程中,随着氧化活性位点的消耗,BC上的DTT活性降低。

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