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化学进展 2023, Vol. 35 Issue (9): 1313-1326 DOI: 10.7536/PC221201 前一篇   后一篇

• 综述 •

PM2.5中二次硫酸盐和硝酸盐生成机制

郭方方, 谢绍东*()   

  1. 北京大学环境科学与工程学院 北京 100871
  • 收稿日期:2022-12-28 修回日期:2023-08-16 出版日期:2023-09-24 发布日期:2023-08-23
  • 作者简介:

    谢绍东 北京大学教授、博士生导师,主要从事城市与区域大气污染成因、来源与控制及区域大气污染综合治理规划等研究,负责完成了国家重点基础研究发展计划(973计划)、国家高技术研究发展计划(863计划)、国家重点研发计划和总理基金大气重污染成因与治理攻关等多项科研项目。建立的挥发性有机物排放源清单编制方法体系被生态环境部作为技术规范在全国颁布实施。曾获首都环境保护先进个人,省部级科技进步一、二等奖共11项以及国家科学技术进步二等奖。

  • 基金资助:
    国家重点研发计划项目(2018YFC0214001)
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Formation Mechanisms of Secondary Sulfate and Nitrate in PM2.5

Fangfang Guo, Shaodong Xie()   

  1. College of Environmental Sciences and Engineering, Peking University,Beijing 100871, China
  • Received:2022-12-28 Revised:2023-08-16 Online:2023-09-24 Published:2023-08-23
  • Contact: *e-mail: sdxie@pku.edu.cn
  • Supported by:
    The National Key Research and Development Program of China(2018YFC0214001)

二次无机硫酸盐和硝酸盐是PM2.5的关键化学组分,对区域霾污染的形成有十分重要的作用。厘清两者的生成机制对于消除PM2.5污染至关重要。二次硫酸盐和硝酸盐的生成机理十分复杂,包括气相、液相和非均相等多种反应。最近的实验和观测研究揭示了SO2和NO2生成硫酸盐和硝酸盐的新机理和详细的反应动力学,其被用于空气质量模型后可有效提升数值模式对硫酸盐和硝酸盐的时空分布特征及生成过程的模拟。本文系统总结了PM2.5中二次硫酸盐和硝酸盐生成机制的最新进展,重点阐述了SO2和NO2氧化生成硫酸盐和硝酸盐的重要反应途径的机理和反应动力学结果,讨论了影响SO2和NO2氧化速率的因素以及在表征反应动力学时出现的重大实验挑战,同时探讨了硝酸盐对氮氧化物(NOx)、挥发性有机物(VOCs)、氨(NH3)减排的敏感性。最后,对未来研究发展方向提出了建议。

关键词： 硝酸盐, 硫酸盐, 生成机制, 气溶胶液态水含量, 气溶胶酸度

Secondary inorganic sulfate and nitrate, as the key chemical components of PM2.5, play important roles in the formation of severe regional haze events. The deteriorating sulfate and nitrate pollution has brought more serious challenges to the continuous improvement of air quality. Thus, elucidating the formation pathways and key factors of controlling the formation of inorganic sulfate and nitrate is crucial to eliminate PM2.5 pollution in the atmosphere. The formation of sulfate and nitrate involves complex chemical reactions, including gas- and aqueous-phase reactions and multi-phase reactions. Recent experimental and filed studies have revealed new reaction mechanisms and detailed reaction kinetics for the oxidation of SO2 and NO2 to form sulfate and nitrate. Merging new formation pathways of sulfate and nitrate with updating reaction kinetics based on laboratory measurements and field observations, air quality model performance is effectively improved to capture the spatial-temporal variations of sulfate and nitrate and identify their chemical formation pathways. This review provides a synthetic synopsis of recent advances in the fundamental mechanisms of sulfate and nitrate formation. In particular, the mechanisms and reaction kinetic results for a series of individual reaction pathways of current interest for the SO2 and NO2 oxidation are emphasized. The key factors affecting the SO2 and NO2 oxidation rates and significant challenges in laboratory studies of characterizing the reaction kinetics are also discussed. In addition, the sensitivity of nitrate to emission reductions of nitrogen oxides (NOx), volatile organic compounds (VOCs) and ammonia (NH3) is investigated. Finally, suggestions are put forward for the future research directions to improve the understanding of sulfate and nitrate formation.

Contents

1 Introduction

2 Mechanism of particulate sulfate formation

2.1 Gas-phase oxidation

2.2 Aqueous-phase oxidation

2.3 Heterogeneous oxidation

2.4 Multiphase photochemical oxidation

3 Mechanism of particulate nitrate formation

3.1 HNO3 formation

3.2 HNO3-NO3- partitioning

4 Conclusion and outlook

Key words: nitrate, sulfate, formation mechanism, aerosol liquid water content, aerosol acidity
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表1 HNO3生成的主要化学反应
Table 1 The main reactions contributing to HNO3 formation
Type Reactions No.
Gas-phase
reactions		 N O 2 + O H → H N O 3 R1
N O 3 + H C → H N O 3 + p r o d u c t s R2
N O + H O 2 / R O 2 → H N O 3 ( g ) R3
Heterogeneous
reactions		 N O 2 + N O 3 → N 2 O 5 N 2 O 5 + H 2 O → 2 H N O 3 ( a q ) R4
N O 2 + N O 3 → N 2 O 5 N 2 O 5 + C l - → C l N O 2 + N O 3 - ( a q ) R5
2 N O 2 + H 2 O → H N O 3 + H O N O R6
N O 2 + X O → X N O 3 , X N O 3 + H 2 O → H N O 3 ( a q ) R7
N O 3 + H 2 O → H N O 3 ( a q ) R8
N O 3 + M T N / I S O P → R O N O 2 R O N O 2 + H 2 O → H N O 3 ( a q ) R9
N O + R O 2 → R O N O 2 R O N O 2 + H 2 O → H N O 3 ( a q ) R10
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