2014年夏季华北平原郊区站点(望都)ROx自由基的观测和模拟
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- 英文论文题名：Observation and modelling of the RO_X radicals at a rural site(Wangdu) in the North China Plain in summer 2014
- 论文作者：陆克定 ; 张远航 ; 谭照峰 ; 曾立民 ; 刘禹含 ; Hendirk Fuchs ; Andreas Hofzumahaus ; Frank Holland ; Xin Li ; Andreas Wahner
- 英文论文作者：Keding Lu ; Yuanhang Zhang ; Zhaofeng Tan ; Limin Zeng ; Yuhan Liu ; Hendrik Fuchs ; Andreas Hofzumahaus ; Frank Holland ; Xin Li ; Andreas Wahner ; College of Environmental Sciences and Engineering ; Peking University ; Institute of Energy and Climate Research ; IEK-8 ; Troposphere ; Forschungszentrum Juelich GmbH
- 年：2016
- 作者机构：北京大学环境科学与工程学院;Institute of Energy and Climate Research,IEK-8:Troposphere,Forschungszentrum Juelich GmbH;
- 论文关键词：激光诱导荧光 ; OH自由基 ; HO2自由基 ; RO2自由基 ; HONO
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第二十六分会：环境化学
- 语种：中文
- 分类号：X51
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第二十六分会 ; 环境化学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：122k
- 原文格式：D
- 会议级别：全国
摘要
对大气氧化性普遍规律的认识,是理解臭氧和灰霾污染及全球辐射收支等重大环境问题的理论基础。ROx(=OH+HO~(2+)RO2)自由基化学作为对流层大气氧化能力的主要构成部分,其反应机理一直是国际大气化学研究的热点和前沿。基于自由基收支闭合实验思想,搭建了北京大学大气激光诱导荧光系统,在华北平原典型郊区站点开展了包含自由基直接准确测量的综合外场观测。观测结果显示华北平原存在高浓度自由基,OH、HO2、RO2的日间峰值浓度水平分别可达(5-15)×106cm-3,(3-14)×108 cm-3 and(3-15)×108 cm-3。使用基于观测的模型进行分析发现,目前最先进的大气化学机理在高VOCs和低NOx条件下仍然低估OH观测结果2倍左右。与之前珠三角和北京地区观测发现类似,向模型中引入"OH自由基非传统再生机制"可以实现对OH的准确模拟。此外,模型在清晨时段显著低估了RO2自由基观测结果,这说明清晨时段RO2自由基存在未知来源机制;同时这也意味着现有模型对局地臭氧光化学产生速率及其控制区的敏感性分析存在显著偏差。
A comprehensive field campaign was carried out in summer 2014 in Wangdu located in the North China Plain.A month of continuous ROx measurements were obtained by a laser induced fluorescence system.High daytime OH,HO2 and RO2 radical concentrations were observed of which their daily maximum concentrations were(5-15)×106cm-3,(3-14)×108 cm-3 and(3-15)×108 cm-3,respectively.A chemical box model constrained by observed trace gas compounds with state of art chemical mechanism is used to interpret the observed radical concentrations.The model underestimated the observed OH concentrations by a factor of 2 when NO is less than 100 ppt in the afternoon hours.Like PRIDE-PRD and CAREBEIJING,an additional OH recycling is required to reproduce the observed OH concentrations for the high VOC and low NOx conditions.Based on the chemical modulation experiments we performed at the site,the determined OH interference signal were very small for the afternoon conditions.In addition,we found that observed RO2 concentrations were underestimated in the morning hours which indicated the existence of additional chemical sources of RO2 and an underestimation of the local ozone production rates in current model.
A comprehensive field campaign was carried out in summer 2014 in Wangdu located in the North China Plain.A month of continuous ROx measurements were obtained by a laser induced fluorescence system.High daytime OH,HO2 and RO2 radical concentrations were observed of which their daily maximum concentrations were(5-15)×106cm-3,(3-14)×108 cm-3 and(3-15)×108 cm-3,respectively.A chemical box model constrained by observed trace gas compounds with state of art chemical mechanism is used to interpret the observed radical concentrations.The model underestimated the observed OH concentrations by a factor of 2 when NO is less than 100 ppt in the afternoon hours.Like PRIDE-PRD and CAREBEIJING,an additional OH recycling is required to reproduce the observed OH concentrations for the high VOC and low NOx conditions.Based on the chemical modulation experiments we performed at the site,the determined OH interference signal were very small for the afternoon conditions.In addition,we found that observed RO2 concentrations were underestimated in the morning hours which indicated the existence of additional chemical sources of RO2 and an underestimation of the local ozone production rates in current model.
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