大气氧化能力(AOC)通常是指大气通过氧化过程去除大气中微量气体成分的速率总和。在对流层和近地层大气中,AOC主要表观为对污染气体的清除能力或净化能力,亦称大气氧化性。AOC是地球大气自洁净的核心能力,但一直缺乏对其内涵的深入认知...大气氧化能力(AOC)通常是指大气通过氧化过程去除大气中微量气体成分的速率总和。在对流层和近地层大气中,AOC主要表观为对污染气体的清除能力或净化能力,亦称大气氧化性。AOC是地球大气自洁净的核心能力,但一直缺乏对其内涵的深入认知和对其指标的量化描述。本文作者通过承担国家重点研发计划“区域大气氧化能力与空气质量的定量关系及调控原理”研究等项目,从大气化学基本理论入手,对AOC开展了系列研究,并在其量化表达方面取得了突破性进展。本文将围绕“大气氧化能力量化研究”这一科学问题,对这些进展进行简要的描述。首先在深入认知AOC内涵的基础上,分别从大气化学的热力学和动力学基本原理出发,构建了大气氧化能力表观指数(AOIe)和潜势指数(AOIp),并通过二者归一化指数日变化闭合研究,发现了非均相化学过程对AOC的贡献不容忽视。随着PM2.5污染的加重,无论夏季还是冬季,AOIe亦随之增加,但在冬季AOIp则出现了相反的情景,表现出AOIp的变化受气象条件的影响更大。AOC闭合研究思路用于大气OH自由基的储库分子HONO“未知源”研究,发现了北京大气HONO的重要非均相来源,阐释了MCM(Master Chemical Mechanism)机制对冬季AOC低估的重要原因。AOIp用于预测我国大气臭氧污染潜势格局,发现臭氧光化学生成表观潜势(AOIp_O_(3))与NO_(2)的光解系数[J(NO_(2))]直接相关,全国J(NO_(2))的年均值为4.39×10^(-3)s^(-1),高值区主要分布在四川、贵州、重庆和湖南等地。与其他化学反应氧化性指数对比,AOIe与AOIp组合指数更具准确性、普适性和实用性,可评价已发生的污染过程AOC的变化,亦可预测城市或区域重污染发生的可能性及其变化和格局。展开更多
Soil respiration is a main dynamic process of carbon cycle in wetland. It is important to contribute to global climate changes. Water table and nutritious availability are significant impact factors to influence respo...Soil respiration is a main dynamic process of carbon cycle in wetland. It is important to contribute to global climate changes. Water table and nutritious availability are significant impact factors to influence responses of CO2 emission from wetland soil to climate changes. Twenty-four wetland soil monoliths at 4 water-table positions and in 3 nitrogen status have been incubated to measure rates of CO2 emission from wetland soils in this study. Three static water-table controls and a fluctuant water-table control, with 3 nitrogen additions in every water-table control, were carried out. In no nitrogen addition treatment, high CO2 emissions were found at a static low water table (Ⅰ) and a fluctuant water table (Ⅳ), averaging 306.7mg/(m2·h) and 307.89mg/(m2·h), respectively, which were 51%-57% higher than that at static high water table (Ⅱ and Ⅲ). After nitrogen addition, however, highest CO2 emission was found at Ⅱ and lowest emission at Ⅲ. The results suggested that nutritious availability of wetland soil might be important to influence the effect of water table on the CO2 emission from the wetland soil. Nitrogen addition led to enhancing CO2 emissions from wetland soil, while the highest emission was found in 1N treatments other than in 2N treatments. In 3 nutritious treatments, low CO2 emissions at high water tables and high CO2 emissions at low water tables were also observed when water table fluctuated. Our results suggested that both water table changes and nutritious imports would effect the CO2 emission from wetland.展开更多
full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban si...full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.展开更多
文摘大气氧化能力(AOC)通常是指大气通过氧化过程去除大气中微量气体成分的速率总和。在对流层和近地层大气中,AOC主要表观为对污染气体的清除能力或净化能力,亦称大气氧化性。AOC是地球大气自洁净的核心能力,但一直缺乏对其内涵的深入认知和对其指标的量化描述。本文作者通过承担国家重点研发计划“区域大气氧化能力与空气质量的定量关系及调控原理”研究等项目,从大气化学基本理论入手,对AOC开展了系列研究,并在其量化表达方面取得了突破性进展。本文将围绕“大气氧化能力量化研究”这一科学问题,对这些进展进行简要的描述。首先在深入认知AOC内涵的基础上,分别从大气化学的热力学和动力学基本原理出发,构建了大气氧化能力表观指数(AOIe)和潜势指数(AOIp),并通过二者归一化指数日变化闭合研究,发现了非均相化学过程对AOC的贡献不容忽视。随着PM2.5污染的加重,无论夏季还是冬季,AOIe亦随之增加,但在冬季AOIp则出现了相反的情景,表现出AOIp的变化受气象条件的影响更大。AOC闭合研究思路用于大气OH自由基的储库分子HONO“未知源”研究,发现了北京大气HONO的重要非均相来源,阐释了MCM(Master Chemical Mechanism)机制对冬季AOC低估的重要原因。AOIp用于预测我国大气臭氧污染潜势格局,发现臭氧光化学生成表观潜势(AOIp_O_(3))与NO_(2)的光解系数[J(NO_(2))]直接相关,全国J(NO_(2))的年均值为4.39×10^(-3)s^(-1),高值区主要分布在四川、贵州、重庆和湖南等地。与其他化学反应氧化性指数对比,AOIe与AOIp组合指数更具准确性、普适性和实用性,可评价已发生的污染过程AOC的变化,亦可预测城市或区域重污染发生的可能性及其变化和格局。
文摘Soil respiration is a main dynamic process of carbon cycle in wetland. It is important to contribute to global climate changes. Water table and nutritious availability are significant impact factors to influence responses of CO2 emission from wetland soil to climate changes. Twenty-four wetland soil monoliths at 4 water-table positions and in 3 nitrogen status have been incubated to measure rates of CO2 emission from wetland soils in this study. Three static water-table controls and a fluctuant water-table control, with 3 nitrogen additions in every water-table control, were carried out. In no nitrogen addition treatment, high CO2 emissions were found at a static low water table (Ⅰ) and a fluctuant water table (Ⅳ), averaging 306.7mg/(m2·h) and 307.89mg/(m2·h), respectively, which were 51%-57% higher than that at static high water table (Ⅱ and Ⅲ). After nitrogen addition, however, highest CO2 emission was found at Ⅱ and lowest emission at Ⅲ. The results suggested that nutritious availability of wetland soil might be important to influence the effect of water table on the CO2 emission from the wetland soil. Nitrogen addition led to enhancing CO2 emissions from wetland soil, while the highest emission was found in 1N treatments other than in 2N treatments. In 3 nutritious treatments, low CO2 emissions at high water tables and high CO2 emissions at low water tables were also observed when water table fluctuated. Our results suggested that both water table changes and nutritious imports would effect the CO2 emission from wetland.
基金supported by the National Natural Science Foundation of China[grant numbers 42275120 and 42075111]the National Key Research and Development Program[grant number 2023YFC3706101]。
文摘full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.
