Atmospheric reactive nitrogen cycling over the ocean

海洋上空的大气活性氮循环

基本信息

  • 批准号:
    NE/S000518/1
  • 负责人:
  • 金额:
    $ 78.79万
  • 依托单位:
  • 依托单位国家:
    英国
  • 项目类别:
    Research Grant
  • 财政年份:
    2019
  • 资助国家:
    英国
  • 起止时间:
    2019 至 无数据
  • 项目状态:
    已结题

项目摘要

Atmospheric chemical processing drives the removal of emitted pollutants, and leads to the formation of ozone and secondary aerosol, which are harmful to human and environmental health, and contribute to climate forcing. Quantitative understanding of such chemistry is essential for the accurate prediction of current air quality and future atmospheric composition.In the troposphere, gaseous chemical processing is critically dependent upon the abundance of nitrogen oxides (NOx, NO + NO2), which regulate atmospheric oxidising capacity, ozone formation and the major components of many aerosol particles. Globally, the dominant NOx sources are all continental (traffic, power generation, industry, soil emissions of NO); these are well understood in some locations, but are very uncertain and rapidly increasing in developing nations, particularly African megacities. Once in the atmosphere, NOx is converted to reservoir compounds such as PAN, which may release NOx after transport, and ultimately into nitric acid (HNO3) on timescales of days. Current understanding is that HNO3 is the final atmospheric sink for NOx, and is removed from the atmosphere by deposition. Consequently, at remote marine sites a number of days transit time from the coast, we would expect NOx levels to be very low, and the inorganic nitrogen budget to be dominated by unreactive transported HNO3.Recent observations challenge this understanding: surprisingly high levels of NOx species, and HONO (a NOx precursor with a lifetime of a few minutes) have been observed over the tropical Atlantic ocean. This points to a missing source of HONO and NOx. It has been hypothesised that the photolytic conversion of particle-bound nitrate to gaseous HONO and NO2 may account for these observations and form the missing NOx source - a mechanism termed "renoxification" (Ye et al., Nature 2016). We have performed proof-of-concept measurements and modelling of HONO and NOx levels at the Cape Verde observatory in the tropical Atlantic, which we have found to be consistent with this mechanism (Reed et al., ACP, 2017) - however, order of magnitude uncertainties over the rate and products of particle nitrate photolysis remain, and observational evidence for its occurrence on dominant aerosol species (dust, sulfate aerosol) is missing, meaning that impacts on the global-scale are unknown.This project aims to address these uncertainties, through integrating existing ground-based, aircraft and satellite observations with targeted new field and laboratory studies. We will focus upon a natural laboratory, the tropical Atlantic region where we will probe the emissions and evolution of nitrogen species in the outflow of polluted air from the developing regions of West Africa to the clean marine environment of the mid Atlantic (Cape Verde Observatory, CVO). Specifically, we will (1) Use the tropical Atlantic as a natural laboratory to study renoxification during different seasons and aerosol regimes, alongside laboratory studies to parameterise the particulate nitrate photolysis process; (2) integrate this new understanding into a global chemistry-transport model to evaluate the recycling and transformations of NOx during transport, and hence the impacts of these process in the tropical Atlantic ocean, and upon our understanding of atmospheric chemical processing globally.
大气中的化学处理推动了排放污染物的清除,并导致臭氧和二次气溶胶的形成,这对人类和环境健康有害,并导致气候强迫。在对流层中,气态化学过程主要取决于氮氧化物(NOx,NO + NO2)的丰度,氮氧化物调节着大气的氧化能力、臭氧的形成以及许多气溶胶颗粒的主要成分。在全球范围内,主要的氮氧化物来源都是大陆性的(交通、发电、工业、土壤排放的氮氧化物);这些在一些地方是很好理解的,但在发展中国家,特别是非洲的特大城市,非常不确定,而且迅速增加。一旦在大气中,NOx被转化为储库化合物,如PAN,其可在运输后释放NOx,并最终在数天的时间尺度上转化为硝酸(HNO 3)。目前的理解是,HNO 3是NOx的最终大气汇,并通过沉积从大气中去除。因此,在距离海岸数天的远程海洋站点,我们预计NOx水平非常低,并且无机氮收支由未反应的输送HNO 3主导。最近的观测挑战了这种认识:在热带大西洋上观察到了令人惊讶的高水平NOx物质和HONO(一种寿命为几分钟的NOx前体)。这表明HONO和NOx的来源缺失。已经假设,颗粒结合的硝酸盐到气态HONO和NO2的光解转化可以解释这些观察结果并形成缺失的NOx源-一种称为“再氧化”的机制(Ye等人,Nature 2016)。我们已经在热带大西洋的佛得角天文台对HONO和NOx水平进行了概念验证测量和建模,我们发现这与这种机制一致(Reed等人,ACP,2017年)-然而,颗粒硝酸盐光解的速率和产物的数量级不确定性仍然存在,其发生在主要气溶胶物种上的观测证据(灰尘,硫酸盐气溶胶)缺失,这意味着对全球范围的影响是未知的。本项目旨在解决这些不确定性,通过整合现有的地基,飞机和卫星观测,并进行有针对性的新实地和实验室研究。我们将把重点放在一个自然实验室,热带大西洋地区,我们将探测从西非发展中地区到大西洋中部清洁海洋环境的污染空气流出中氮物质的排放和演变(佛得角天文台,CVO)。具体来说,我们将(1)利用热带大西洋作为一个天然实验室,研究不同季节和气溶胶制度下的再氧化作用,同时进行实验室研究,以参数化颗粒硝酸盐光解过程;(2)将这一新的认识纳入全球化学传输模式,以评估氮氧化物在传输过程中的再循环和转化,从而评估这些过程在热带大西洋中的影响,以及我们对全球大气化学过程的理解。

项目成果

期刊论文数量(10)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Airborne observations over the North Atlantic Ocean reveal the importance of gas-phase urea in the atmosphere.
  • DOI:
    10.1073/pnas.2218127120
  • 发表时间:
    2023-06-20
  • 期刊:
  • 影响因子:
    11.1
  • 作者:
    Matthews, Emily;Bannan, Thomas J.;Khan, M. Anwar H.;Shallcross, Dudley E.;Stark, Harald;Browne, Eleanor C.;Archibald, Alexander T.;Mehra, Archit;Bauguittei, Stephane J. -B.;Reed, Chris;Thamban, Navaneeth M.;Wu, Huihui;Barker, Patrick;Lee, James;Carpenter, Lucy J.;Yang, Mingxi;Bell, Thomas G.;Allen, Grant;Jayne, John T.;Percival, Carl J.;McFiggansa, Gordon;Gallaghera, Martin;Coe, Hugh
  • 通讯作者:
    Coe, Hugh
Long-term NO<sub>x</sub> measurements in the remote marine tropical troposphere
长期否
  • DOI:
    10.5194/amt-2020-469
  • 发表时间:
    2020
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Andersen S
  • 通讯作者:
    Andersen S
Is the ocean surface a source of nitrous acid (HONO) in the marine boundary layer?
  • DOI:
    10.5194/acp-2021-532
  • 发表时间:
    2021-07
  • 期刊:
  • 影响因子:
    6.3
  • 作者:
    L. Crilley;L. Kramer;F. Pope;C. Reed;James D. Lee;L. Carpenter;L. Hollis;S. Ball;W. Bloss
  • 通讯作者:
    L. Crilley;L. Kramer;F. Pope;C. Reed;James D. Lee;L. Carpenter;L. Hollis;S. Ball;W. Bloss
Discovering global-scale processes in the marine atmosphere
发现海洋大气中的全球规模过程
  • DOI:
    10.5194/egusphere-egu24-11717
  • 发表时间:
    2024
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Carpenter L
  • 通讯作者:
    Carpenter L
Measurements and experimental budget analysis of OH, HO2 and RO2 radicals in a remote tropical marine location
偏远热带海洋位置 OH、HO2 和 RO2 自由基的测量和实验预算分析
  • DOI:
    10.5194/egusphere-egu24-9483
  • 发表时间:
    2024
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Seldon S
  • 通讯作者:
    Seldon S
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Lucy Carpenter其他文献

Modelling different strategies to prevent coronary heart disease in primary care.
对初级保健中预防冠心病的不同策略进行建模。
  • DOI:
    10.1016/0895-4356(94)90114-7
  • 发表时间:
    1994
  • 期刊:
  • 影响因子:
    7.2
  • 作者:
    C. Silagy;D. Mant;Lucy Carpenter;John Muir;Andrew Neil
  • 通讯作者:
    Andrew Neil
Update on Ozone-Depleting Substances (ODSs) and Other Gases of Interest to the Montreal Protocol, Chapter 1 in Scientific Assessment of Ozone Depletion: 2014, Global Ozone Research and Monitoring Project-Report No.55, 416 pp., World Meteorological Organiz | NIST
《蒙特利尔议定书》中消耗臭氧层物质 (ODS) 和其他相关气体的更新,臭氧消耗科学评估第 1 章:2014 年,全球臭氧研究和监测项目报告第 55 号,第 416 页,世界气象组织 |
  • DOI:
  • 发表时间:
    2014
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Lucy Carpenter;S. Reimann;A. Engel;S. Montzka;J. B. Burkholder;Cathy Clerbaux;B. Hall;Shari A. Yvon;D. R. Blake;M. Dorf;G. Dutton;P. Fraser;Lucien Froidevaux;François Hendrick;Jianxin Hu;Ashley Jones;P. Krummel;L. Kuijpers;M. Kurylo;Qing Liang;Emmanuel Mahieu;Jens M hle;S. O. Doherty;K. Ohnishi;V. L. Orkin;K. Pfeilsticker;Matthew Rigby;I. Simpson;Y. Yokouchi
  • 通讯作者:
    Y. Yokouchi
Overactive bladder: not just a normal part of getting older.
膀胱过度活动症:不仅仅是变老的正常现象。
  • DOI:
  • 发表时间:
    2022
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Lucy Carpenter;N. Campain
  • 通讯作者:
    N. Campain

Lucy Carpenter的其他文献

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{{ truncateString('Lucy Carpenter', 18)}}的其他基金

Iodine sea-air emissions and atmospheric impacts in a changing world (I-SEA)
不断变化的世界中的碘海气排放和大气影响 (I-SEA)
  • 批准号:
    NE/W00027X/1
  • 财政年份:
    2022
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Investigating HALocarbon impacts on the global Environment (InHALE)
调查 HALocarbon 对全球环境的影响 (InHALE)
  • 批准号:
    NE/X003434/1
  • 财政年份:
    2022
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Iodide in the ocean:distribution and impact on iodine flux and ozone loss
海洋中的碘化物:分布及其对碘通量和臭氧损失的影响
  • 批准号:
    NE/N009983/1
  • 财政年份:
    2016
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Oceanic Reactive Carbon: Chemistry-Climate impacts (ORC3)
海洋活性碳:化学-气候影响 (ORC3)
  • 批准号:
    NE/K004980/1
  • 财政年份:
    2013
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Co-ordinated Airborne Studies in the Tropics (CAST)
热带地区协调机载研究 (CAST)
  • 批准号:
    NE/J00619X/1
  • 财政年份:
    2012
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Aerosol-Cloud Coupling And Climate Interactions in the Arctic
北极的气溶胶-云耦合和气候相互作用
  • 批准号:
    NE/I028769/1
  • 财政年份:
    2012
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Doctoral Training Grant (DTG) to provide funding for 1 PhD studentship.
博士培训补助金 (DTG) 为 1 名博士生提供资助。
  • 批准号:
    NE/H527591/1
  • 财政年份:
    2009
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Training Grant
Impact of combined iodine and bromine release on the Arctic atmosphere (COBRA).
碘和溴混合释放对北极大气的影响 (COBRA)。
  • 批准号:
    NE/D006015/1
  • 财政年份:
    2007
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Impact of combined iodine and bromine release on the Arctic atmosphere (COBRA).
碘和溴混合释放对北极大气的影响 (COBRA)。
  • 批准号:
    NE/D006104/1
  • 财政年份:
    2007
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant
Impact of combined iodine and bromine release on the Arctic atmosphere (COBRA).
碘和溴混合释放对北极大气的影响 (COBRA)。
  • 批准号:
    NE/D006287/1
  • 财政年份:
    2007
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Research Grant

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相似海外基金

AGS-PRF: Evaluating the Changing Role of Monoterpenes in Regulating Atmospheric Reactive Nitrogen Budgets
AGS-PRF:评估单萜在调节大气活性氮预算中的作用变化
  • 批准号:
    2132296
  • 财政年份:
    2022
  • 资助金额:
    $ 78.79万
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    Fellowship Award
Exploratory research on new source of atmospheric reactive nitrogen focusing on marine nitrogen-fixing organisms
以海洋固氮生物为重点的大气活性氮新来源探索研究
  • 批准号:
    21K19835
  • 财政年份:
    2021
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    $ 78.79万
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    Grant-in-Aid for Challenging Research (Exploratory)
Collaborative Research: CEDAR--Quantifying the Impact of Radiation Belt Electron Precipitation on Atmospheric Reactive Nitrogen Oxides (NOx) and Ozone (O3)
合作研究:CEDAR——量化辐射带电子沉淀对大气活性氮氧化物 (NOx) 和臭氧 (O3) 的影响
  • 批准号:
    1650738
  • 财政年份:
    2018
  • 资助金额:
    $ 78.79万
  • 项目类别:
    Standard Grant
Collaborative Research: CEDAR--Quantifying the Impact of Radiation Belt Electron Precipitation on Atmospheric Reactive Nitrogen Oxides (NOx) and Ozone (O3)
合作研究:CEDAR——量化辐射带电子沉淀对大气活性氮氧化物 (NOx) 和臭氧 (O3) 的影响
  • 批准号:
    1650918
  • 财政年份:
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  • 资助金额:
    $ 78.79万
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Development of measurement method and deposition estimation for atmospheric reactive nitrogen in Japan
日本大气活性氮测量方法和沉降估算的发展
  • 批准号:
    15K00529
  • 财政年份:
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  • 资助金额:
    $ 78.79万
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    Grant-in-Aid for Scientific Research (C)
The chemistry, sources and sinks of atmospheric reactive nitrogen
大气活性氮的化学性质、来源和汇
  • 批准号:
    340997-2011
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  • 资助金额:
    $ 78.79万
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    Discovery Grants Program - Individual
The chemistry, sources and sinks of atmospheric reactive nitrogen
大气活性氮的化学性质、来源和汇
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  • 资助金额:
    $ 78.79万
  • 项目类别:
    Discovery Grants Program - Individual
The chemistry, sources and sinks of atmospheric reactive nitrogen
大气活性氮的化学性质、来源和汇
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    340997-2011
  • 财政年份:
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  • 资助金额:
    $ 78.79万
  • 项目类别:
    Discovery Grants Program - Individual
The chemistry, sources and sinks of atmospheric reactive nitrogen
大气活性氮的化学性质、来源和汇
  • 批准号:
    340997-2011
  • 财政年份:
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  • 资助金额:
    $ 78.79万
  • 项目类别:
    Discovery Grants Program - Individual
The chemistry, sources and sinks of atmospheric reactive nitrogen
大气活性氮的化学性质、来源和汇
  • 批准号:
    340997-2011
  • 财政年份:
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  • 资助金额:
    $ 78.79万
  • 项目类别:
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