ICOZA: Integrated Chemistry of Ozone in the Atmosphere

Lead Research Organisation: University of Birmingham
Department Name: Sch of Geography, Earth & Env Sciences

Abstract

Tropospheric ozone is an important air pollutant, harmful to human health, agricultural crops and vegetation. It is the main precursor to the atmospheric oxidants which initiate the degradation of most reactive gases emitted to the atmosphere, and is an important greenhouse gas in its own right. As a consequence of this central role in atmospheric chemistry and air pollution, the capacity to understand, predict and manage tropospheric ozone levels is a key goal for atmospheric science research. This goal is hard to achieve, as ozone is a secondary pollutant, formed in the atmosphere from the complex oxidation of VOCs in the presence of NOx and sunlight, and the timescale of ozone production is such that a combination of in situ chemical processes, deposition and transport govern ozone levels. Uncertainties in all of these factors affect the accuracy of numerical models used to predict current and future ozone levels, and so hinder development of optimal air quality policies to mitigate ozone exposure. Here, we will address this problem by measuring the local chemical ozone production rate, and (for the first time) perform measurements of the response of the local atmospheric ozone production rate to NOx and VOC levels - directly determining the ozone production regime.

We will achieve this aim by building upon an existing instrument for the measurement of atmospheric ozone production rates (funded through a NERC Technology Proof-of-Concept grant, and deployed in the recent ClearfLo "Clean Air for London" NERC Urban Atmospheric Science programme). In addition to directly measuring ozone production, by perturbing the ambient chemical conditions (for example, through addition of NOx or VOCs to the sampled airflow), and measuring the effect of this change upon the measured ozone production rate, the ozone control regime (extent of NOx vs VOC limitation) may be directly determined. Within this project, we will develop our existing ozone production instrument to include this capability, and validate the measurements, through comparison with ozone production from VOC oxidation in a large simulation chamber, and by measurement of the key oxidant OH radicals, and their precursors, within the system.

We will then apply the instrument to compare the measured ozone production rates with those calculated using other observational and model approaches, and to characterise the ozone control regime, in two contrasting environments: In the outflow of a European megacity (at Weybourne Atmospheric Observatory, WAO, in the UK), and in a rural continental location (at Hohenpeissenberg, HPB, in southern Germany). At WAO, we will compare the measured ozone production rate with that calculated through co-located measurements of HO2 and RO2 radicals (using a newly developed approach to distinguish between these closely related species), and with that simulated using a constrained photochemical box model. We will compare the NOx-dependence of the ozone production rate with that predicted using indicator approaches, based upon observations of other chemical species. At HPB, we will focus upon the VOC-dependence of the ozone production rate, and assess the error in model predictions of ozone production, which arise from the presence of unmeasured VOCs.

The project will develop and demonstrate a new measurement approach, and apply this to improve our understanding of a fundamental aspect of atmospheric chemical processing. Future applications have considerable potential both to support atmospheric science research, but also as an important air quality tool, alongside existing measurement and modelling approaches, to inform the most effective emission controls to reduce ozone production in a given location. In the context of global crop yield reductions arising from ozone exposure of 7 - 12 % (wheat), 6 - 16 % (soybean) and 3 - 4 % (rice), this is an important societal as well as scientific goal.

Planned Impact

Impact Summary

The project will deliver new scientific insight into our current understanding of atmospheric ozone formation, and quantify the systematic errors present in model predictions of ozone formation from unmeasured species and/or incomplete chemical understanding. It will also provide a new measurement capability to quantify local ozone production rates, and to directly establish the prevailing ozone control regime. Accordingly we identify two key groups of immediate beneficiaries

-Research scientists studying all aspects of atmospheric ozone chemistry, and impacts of ozone upon climate, vegetation and human health.

-The air quality community, and policy makers involved in the development and formulation of air pollution control measures.

We will ensure the impact of the project to these groups is maximised through the following specific activities, alongside traditional dissemination routes (conferences, journal publications) :

(1) Direct liaison with the relevant atmospheric science research community, leveraging the PIs ongoing links to a range of relevant projects and groupings such as NCAS, TF HTAP

(2) Direct dissemination of the project results, and new measurement capability, to the Air Quality community, through our links to bodies such as AQEG

(3) By holding a focussed discussion workshop on the topic of "Local Chemical Ozone Production" disseminate the project science outcomes, leading to the preparation of a position paper reviewing the state of our understanding in this area.

(4) By convening a forum for the knowledge exchange over capabilities and needs in atmospheric measurement, between the atmospheric science research community, air quality monitoring practitioners, and those at the interface between atmospheric research and air quality policy, supported by the IAQM and learned societies.

Wider Beneficiaries: Scientific Community; General Public
The research proposed here will lead, both directly and through improved general scientific understanding, to improved ozone control strategies / policies. This will benefit the general public, as tropospheric ozone is a key pollutant, harmful to health, reducing crop yields, damaging materials and contributing to climate change. The outcomes of this work will therefore address two of the key RCUK definitions of impact, namely "increasing the effectiveness of public policy" and "enhancing quality of life and health".

Publications

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Description Tropospheric ozone is a major air pollutant, harmful to human health, agricultural crops and vegetation, the main precursor to the atmospheric oxidants which initiate the degradation of most reactive gases emitted to the atmosphere, and an important greenhouse gas in its own right. The capacity to understand, predict and manage tropospheric ozone levels is a key goal for atmospheric science - but one which is hard to achieve, as ozone is formed in the atmosphere from the complex oxidation of VOCs in the presence of NOx and sunlight, on a timescale such that in situ chemical processes, deposition and transport all affect ozone levels, reflected in the continuity equation for boundary layer ozone (below). Known uncertainties in emissions, chemistry, dynamics and deposition affect the accuracy of predictions of current and future ozone levels, and hinder development of optimal air quality policies to mitigate against ozone exposure.

The aim of this project is to apply an innovative solution to the chemical aspect of this critical problem: To develop, refine and apply in situ measurements of the local chemical ozone production rate, and to make the first measurements of the response of the ozone production rate to NOx and VOC level. This approach will implicitly integrate the full atmospheric chemical complexity, hence avoid limitations inherent in emissions inventories and chemical mechanisms, and explicitly distinguish between the chemical and dynamical factors controlling local ozone production.

We have developed a new instrument for the measurement of ozone production rates (funded through a NERC Technology Proof-of-Concept grant) to improve its performance, and added the capability to measure the ozone control regime. We have applied the instrument to compare measured ozone production rates with those calculated using other observational and model approaches, to characterise the ozone control regime with respect to NOx in the outflow of a European megacity - through a major field campaign at Weybourne Atmospheric Observatory in July 2015.

While the instrument was in part successful, in particular during the highest ozone episode observed in 2015, it has not proved sufficiently sensitive to distinguish more routin ozone chemistry from instrumental background. Ongoing analysis of results from the campaign will focus upon looking at ozone production rates and formation chemical regimes derived from (novel) measurements of OH, HO2 and RO2 radicals performed by the FAGE approach, rather than the OPR instrument.
Exploitation Route Project results have been incorporated in follow-on projects - APHH-China
Sectors Environment

 
Description NERC Internation Opportunities FUnd
Amount £47,971 (GBP)
Funding ID NE/M00581X/1 
Organisation Natural Environment Research Council 
Sector Public
Country United Kingdom
Start 01/2015 
End 12/2016
 
Title NOx interference data 
Description  
Type Of Material Database/Collection of data 
Year Produced 2020 
Provided To Others? Yes  
URL http://edata.bham.ac.uk/566/