Critical Roles of Surface-Enhanced Heterogeneous Oxidation of SO2 in Haze Chemistry: Review of Extended Pathways for Complex Air Pollution

IF 6.4 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Current Pollution Reports Pub Date : 2024-01-12 DOI:10.1007/s40726-023-00287-2
Zihao Zhang, Haiwei Li, Wingkei Ho, Long Cui, Qihui Men, Li Cao, Yunjiang Zhang, Junfeng Wang, Cheng Huang, Shun-cheng Lee, Yu Huang, Mindong Chen, Xinlei Ge
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Abstract

Purpose of Review

Complex air pollution has spread in the conurbation areas of China along with chemically complicated air pollution processes. Classic secondary-pollutant formation toward high concentrations of fine particulate matter (PM2.5) and ozone (O3) is imperfectly understood in the currently accepted chemical mechanisms. The combustion-produced fine particles contain abundant nanosized black carbon (BC) internally mixed with transition metal ions (TMI) and contribute to the complicated oxidation pathways and products substantially. Based on current understandings of multiphase sulfate formation, we propose that the surface-enhanced heterogeneous reaction processes can play critical roles in the fast formation of “haze chemistry smog” pollution.

Recent Findings

Pathways of sulfate enhancement by BC and TMI have been identified to explain the formation mechanisms of the missing sulfate sources. Responsible for additional production of secondary gas molecules and aerosols, the heterogeneous chemistry is initiated with surface photosensitive catalysis. In addition, unidentified atmospheric oxidizing capacity is recognized as part of the heterogeneous processes. Given unique surface-specific profiles and electronically excited dismutation reactions, BC and TMI particles can steadily generate reactive oxygen species (ROS) such as hydroxyl radicals (OH) and promote the oxidation of SO2. This phenomenon provides an extended insight into atmospheric free-radical chemistry. As such, the heterogeneous catalytic oxidation of SO2 on aerosol surfaces accounts for up to 69.2% of sulfate formation in haze episodes.

Summary

Unlike in-cloud aqueous oxidation, representative heterogeneous reaction pathways (i.e., TMI aqueous catalysis pathway and surface catalysis pathway) enhance sulfate formation via surface radical reactions in both winter and summer. The heterogeneous processes are thought to reduce gaps between model-predicted and measured sulfate levels. The physically and chemically active BC and TMI can change the composition, morphology, hygroscopicity, and optical properties of PM in their atmospheric aging processes. Therefore, the heterogeneous pathways facilitate rapid particle growth for haze pollution and help to understand and develop a new type of air pollution chemistry (i.e., “haze chemistry” processes) in China and other developing countries.

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二氧化硫的表面强化异相氧化在灰霾化学中的关键作用:回顾复杂空气污染的扩展途径
综述目的伴随着复杂的空气污染化学过程,复杂的空气污染已在中国城市群地区蔓延。对于高浓度细颗粒物(PM2.5)和臭氧(O3)等典型二次污染物的形成,目前公认的化学机制尚不完善。燃烧产生的细颗粒物含有大量纳米级黑碳(BC),内部混杂着过渡金属离子(TMI),对复杂的氧化途径和产物起着重要作用。基于目前对多相硫酸盐形成的理解,我们提出表面增强的异相反应过程在 "雾霾化学烟雾 "污染的快速形成过程中起着至关重要的作用。通过表面光敏催化作用启动的异相化学反应负责产生额外的二次气体分子和气溶胶。此外,未识别的大气氧化能力也被认为是异相过程的一部分。鉴于独特的表面特异性剖面和电子激发的歧化反应,BC 和 TMI 粒子可以稳定地产生活性氧(ROS),如羟基自由基(OH),并促进二氧化硫的氧化。这一现象为大气自由基化学提供了一个扩展的视角。因此,气溶胶表面 SO2 的异相催化氧化占雾霾事件中硫酸盐形成的 69.2%。摘要与云内水氧化不同,代表性的异相反应途径(即 TMI 水催化途径和表面催化途径)在冬季和夏季都会通过表面自由基反应促进硫酸盐的形成。异相过程被认为可以缩小模型预测与测量的硫酸盐水平之间的差距。具有物理和化学活性的 BC 和 TMI 可在大气老化过程中改变可吸入颗粒物的成分、形态、吸湿性和光学特性。因此,异构途径可促进灰霾污染颗粒物的快速增长,并有助于理解和发展中国和其他发展中国家的新型空气污染化学过程(即 "灰霾化学 "过程)。
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来源期刊
Current Pollution Reports
Current Pollution Reports Environmental Science-Water Science and Technology
CiteScore
12.10
自引率
1.40%
发文量
31
期刊介绍: Current Pollution Reports provides in-depth review articles contributed by international experts on the most significant developments in the field of environmental pollution.By presenting clear, insightful, balanced reviews that emphasize recently published papers of major importance, the journal elucidates current and emerging approaches to identification, characterization, treatment, management of pollutants and much more.
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