Science of the Total Environment 701 (2020) 134463

Contents lists available at ScienceDirect

Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Review

Statistical spatial-temporal modeling of ambient ozone exposure for

environmental epidemiology studies: A review
Runmei Ma, Jie Ban, Qing Wang, Tiantian Li ⇑
National Institute of Environmental Health, Chinese Center for Disease Control and Prevention, No. 7, Panjiayuan Nanli, Chaoyang District, Beijing 100021, China

h i g h l i g h t s g r a p h i c a l a b s t r a c t

 Comprehensively reviewed main

statistical models for ambient ozone
exposure assessment.
 Advantages and disadvantages of the
above models were summarized.
 Suggestions on future application of
these models in environmental
epidemiology were provided.

a r t i c l e i n f o a b s t r a c t

Article history: Background: Studies have discovered the adverse health impacts of ambient ozone. Most epidemiological
Received 29 June 2019 studies explore the relationship between ambient ozone and health effects based on fixed site monitoring
Received in revised form 28 August 2019 data. Fine modeling of ground-level ozone exposure conducted by statistical models has great advantages
Accepted 13 September 2019
for improving exposure accuracy and reducing exposure bias. However, there is no review summarizing
Available online 5 October 2019
such studies.
Guest editor: Pavlos Kassomenos Objectives: A review is presented to summarize the basic process of model development and to provide
some suggestions for researchers.
Keywords:
Methods: A search of PubMed, Web of Science and the Wanfang Database was performed for dates
Ambient ozone through July 1, 2019 to obtain relevant studies worldwide. We also examined the references of the arti-
Statistical model cles of interest to ensure that as many articles as possible were included.
Exposure assessment Results: The land use regression model (LUR model), random forest model and artificial neural network
Environmental epidemiology model have been used in this field. We summarized these studies in terms of model selection, data prepa-
ration, simulation scale selection, and model establishment and validation. Multiparameters are a major
feature of models. Parameters that influence the formation of ground-level ozone concentrations and
parameters that have been extremely important in previous articles should be considered first. The pro-
cess of model establishment and validation is essentially a process of continuously optimizing the model
performance, but there are certain differences in the specific models.
Conclusion: This review summarized the basic process of the statistical model for ambient ozone expo-
sure. We gave the applicable conditions and application scope of different models and summarized the
advantages and disadvantages of various models in ozone modeling research. In the future, research is
still needed to explore this area based on its own research purposes and capabilities.
Ó 2019 Elsevier B.V. All rights reserved.

⇑ Corresponding author.
E-mail address: litiantian@nieh.chinacdc.cn (T. Li).

https://doi.org/10.1016/j.scitotenv.2019.134463
0048-9697/Ó 2019 Elsevier B.V. All rights reserved.
2 R. Ma et al. / Science of the Total Environment 701 (2020) 134463

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Results. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.1. Land use regression model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2. Random forest model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.3. Artificial neural network model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
4. Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
4.1. Model selection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4.2. Data preparation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4.2.1. Monitoring data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4.2.2. Parameter selection and preparation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4.3. Simulation scale determination . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
4.4. Model development and validation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
4.5. Application of the simulation results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
4.6. Prospects and limitations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
5. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

1. Introduction and to provide suggestions for future studies. We will provide a

brief introduction of the models mostly used in this field. In this
As a secondary air pollutant, ambient ozone is a concern due to review, four factors will be considered: model selection, data
its widespread pollution (Anenberg et al., 2010). The adverse preparation, simulation scale determination, and model develop-
health effects of ground-level ozone have been proven by many ment and validation. Applications and limitations will also be
international studies, and the outcomes have showed varied discussed.
effects, such as the mortality of all non-accidental causes, cardio-
vascular, respiratory and coronary diseases, and hypertension
2. Methods
(Yin et al., 2017; Bell, 2004; Wong et al., 2008; Peng et al., 2013;
Di et al., 2017b; Yang et al., 2017). The harmful effects of ozone
To include a wide range of relevant studies, we searched impor-
have also been tested at more sophisticated levels by using, for
tant databases in English and Chinese, including PubMed, Web of
example, glucose (Yang et al., 2018), blood pressure (Cole-Hunter
Science and the Wanfang Database. The search was performed
et al., 2018) and inflammatory markers (Lee et al., 2018). Therefore,
for dates through July 1, 2019 to obtain relative studies worldwide.
ambient ozone causes serious public health problems. Exposure
The search words included were ‘‘ozone”, ‘‘O3”, ‘‘estimate”, ‘‘pre-
assessments of ozone are key to exploring the relationship
dict”, ‘‘forecast”, ‘‘spatiotemporal”, ‘‘spatial”, and ‘‘temporal”,
between ambient ozone and health.
which were searched in both English and Chinese. We also exam-
For environmental epidemiological studies that focus on the
ined the references of the articles of interest to ensure that as many
health effects caused by ambient ozone, there is a great demand
articles as possible were included.
for the accurate assessment of ambient ozone exposure. For long-
The exclusion criteria for the review are as follows: 1) studies
term exposure studies, high-resolution exposure data for historical
that do not mainly rely on mathematical statistics theories, such
periods were sparse, while for short-term exposure studies, many
as chemical transport models (CTMs) and air quality models; 2)
regions lack continuous daily ozone data from monitoring sites.
unspecified descriptions of the parameters and conducting process
Monitoring data have been commonly used in previous studies,
and unclear results; and 3) literature with repeated reports (Fig. 1).
but they are insufficient at the spatial and temporal scales and thus
result in incomplete exposure assessment. Even when the monitor-
ing data are complete, using the data to represent personal expo-
sure results in errors caused by the low precision of instruments
or the gap between averaged individual exposure and the true level
of air pollutants. Some studies further improved exposure accuracy
by matching monitoring data based on home address, but Berkson
error still exists due to differences between personal exposure
level and averaged individual exposure measurements. To solve
the above problems, some studies have explored the use of models
to estimate ground-level ozone exposure at high spatial and tem-
poral resolutions to try to avoid exposure assessment errors as
much as possible. In recent years, focusing on the adverse health
impacts of ozone and the accumulation of various data (satellite
data, chemical transport modeling data, etc.), studies have used
multiparameter statistical models to simulate ground-level ozone
exposure, and the results have been applied to epidemiological
studies; however, a review of these studies has not been
conducted.
The objectives of this review are to discuss recent ground-level
ozone statistical models for environmental epidemiology studies Fig. 1. The study selection process.
Table 1
Details of the studies included in this review.

Authors (year) Study location Study period Temporal Spatial Model Parameters Results
resolution resolution
1 Zhan et al. (2018) China 2015 Daily 0.1°  0.1° Random frost model Atmospheric pressure, evaporation, precipitation, R2 = 0.69;
maximum relative humidity, sunshine duration, temperature, RMSE = 26 mg/m3
8 h mean wind speed, planetary boundary layer height,
elevation, anthropogenic emission inventory, land
use, normalized difference vegetation index (NDVI),
road density, and population density
2 Di et al. (2017) America 2000-2012 Daily 1 km  1 km Neural network Satellite ozone measurements, CTM output, air R2 = 0.76 (0.74–0.80).
maximum 8h temperature, accumulated total precipitation,
mean downward shortwave radiation flux, accumulated
total evaporation, planetary boundary layer height,
low cloud area fraction, precipitation rate,
precipitable water for the entire atmosphere,
pressure, specific humidity at 2 m, visibility, wind
speed, medium cloud area fraction, high cloud area
fraction, albedo, ndvi and vegetation percentage

R. Ma et al. / Science of the Total Environment 701 (2020) 134463

3 Wang et al. (2015) Six metropolitan 1999-2013 Average two- 50 m  50 m LUR with universal Traffic, industrial and port emissions, population city R2: 0.65–0.88; local
areas in America week kriging density, land use and land cover, annual average of R2: 0.60–0.91
concentration specific emission sources
4 Malmqvist et al. (2014) Umeå and Malmö, 2012 Daily average – LUR and temporal Traffic data, land use data, population density, For Malmö, adjusted
Sweden model altitude, wind speed, wind direction, global R2 = 0.40 and CV
radiation, net radiation, temperature, vertical R2 = 0.17. For Umeå,
temperature difference (2–8 m) and vertical adjusted R2 = 0.67 and
temperature difference (24–8 m) CV adjusted R2 = 0.48.
5 Adam-Poupart et al. (2014) Quebec, Canada 2005 8-hr midday 1 km  1 km LUR mixed-effects Temperature, precipitation, days, years, road BME-LUR:
concentration model, Bayesian density and latitude; RMSE = 7.06 ppb,
maximum entropy R2 = 0.653; LUR:
model and kriging R2 = 0.466,
method model RMSE = 8.747; BME
kriging R2 = 0.414,
RMSE = 9.164
6 Kerckhoffs et al. (2015) Netherlands 2012: 2.28–3.15; 4.24– Average of 50  50 m LUR Traffic intensity, length of major roads, low density Summer: R2 = 0.71
5.10; 9.4–9.20; 11.28– the summer residential land, urban green, region annual; R2 = 0.77
12.14 and annual
period
7 Beelen et al. (2009) Europe 2001 Annual 1 km  1 km LUR Land use data, road traffic, population density, R2 = 0.70; RMSE = 7.69
average meteorology, altitude, distance from the ocean.
8 Wang et al. (2016) Los Angeles Basin, 2000–2008 Average two- 4  4 km LUR CTM data, road networks, industrial and port Local: RMSE = 4.56,
America week emissions, population density, land use R2 = 0.78
concentration Routine monitoring and
fixed sites: RMSE = 5.64,
R2 = 0.86
9 Wolf et al (2017) Augsburg, 2014.3-2015.4 Annual 1 km  1 km LUR Local land use, building density, population density, R2 = 0.92
Germany average household density, topography, coordinates, traffic
variables, road network
10 Son et al. (2018) Metropolitan area 2011, 2014 Hourly and 30 m  30 m LUR Temperature, humidity, precipitation, wind speed Hourly R2 = 0.653;
of Mexico monthly and hourly traffic density variables, elevation Monthly R2 = 0.719
11 De Hoogh et al. (2018) Western Europe 2010 Annual 100 m  100 m LUR CTM data, all roads, major roads, ports area, Annual model: R2 = 0.63;
average residential land cover, altitude, north-south trend, warm model: R2 = 0.44;
east-west trend, MACC dispersion model product, cold model: R2 = 0.67
natural land, total build up, urban green
12 Huang et al. (2017) Nanjing, China 2013 Annual 100  100 m LUR Longitude and slope R2 = 0.65
average

3
4 R. Ma et al. / Science of the Total Environment 701 (2020) 134463
3. Results
Based on a preliminary analysis of the literature, we found three
types of models that have been widely used: the land use regres-
sion model (LUR model), the random forest model and the artificial
neural network model. Detailed information of the studies
included in the review is shown in Table 1.
3.1. Land use regression model
The LUR model is a multivariate regression model estab-
lished by the least squares method to simulate the spatial dis-
tribution of the air pollutant concentrations in the study area.
The model integrates land use data and traffic and population
density data around the monitoring site into the geographic
information system (GIS) to analyze the relationship between
these parameters and the spatial distribution of pollutant con-
centrations to estimate the concentration at any location that
does not have monitoring data (Wu et al., 2016). The variables
are generated by setting an increasing buffer distance and
selected according to the backward algorithm and the forward
algorithm. Based on pollutant concentrations and geographic
variables, a multivariate regression model was established by
the least squares method.
LUR models were introduced in the air pollution modeling field
in 1997 (Briggs et al., 1997), and they are normally used in regres-
sion mapping for ambient particulate matter, NOx or VOCs (Hoek
et al., 2008). To the best of our knowledge, the earliest studies
using LUR models to simulate ambient ozone exposure were con-
ducted in 2009 (Beelen et al., 2009). For the spatial scale, in some
ways, LUR models mainly focus on a certain city or region, such as
Quebec (Adam-Poupart et al., 2014) in Canada or metropolitan
areas in the United States (Wang et al., 2015). However, some stud-
ies have modeled ground-level ozone exposure at a broader scale,
such as Beelen et al. (2009), which was conducted in Europe. For
the temporal scale, studies that have focused on long-term expo-
sure are generally based on the annual mean value (Beelen et al.,
2009; Kerckhoffs et al., 2015; Wolf et al., 2017; De Hoogh et al.,
2018; Huang et al., 2017), and studies that have focused on
short-term exposure have scattered hourly values (Son et al.,
2018), 8-h averages (Adam-Poupart et al., 2014), daily means
(Malmqvist et al., 2014) and two-week concentrations (Wang
et al., 2015, 2016). Most LUR models applied in large metropolitan
areas with high spatial resolutions (Hoek et al., 2008), such as the
studies of the metropolitan areas of Mexico City, with a resolution
of 30 m  30 m (Son et al., 2018), or Wang et al. (2015)’s research,
which was based on six metropolitan areas in America and used a
resolution of 50 m  50 m. According to the parameters used in
various studies, commonly used parameters include land use term,
traffic density, population density, emissions inventory and mete-
orological parameters. Most studies evaluated the performance of
the model through the correlation coefficient (R2) or root mean
square error (RMSE). The performances were generally good, with
R2 values up to 0.92 (Augsburg, Germany, 1 km  1 km, hourly)
(Wolf et al., 2017). The LUR model has been widely used in expo-
sure assessments in Europe and North America, and the simulation
results have been used in epidemiological studies (Holle et al.,
2005).
3.2. Random forest model
The random forest model is an algorithm based on a classifica-
tion tree composed of a tree classifier {h (x, H k), k = 1. . .}, where
{H k} is an independent identical distribution random vector and
each tree votes on x. The final results are obtained by averaging
the prediction results of the regression tree for multiple subsample
sets through several rounds of training (Yang, 2014).
Random forest models have been widely used to simulate the
spatial and temporal distributions of air pollutants (Hu et al.,
2017; Zhan et al., 2017), but few studies have used random forest
models in ambient ozone exposure simulations. Zhan et al. (2018)
assessed the ambient ozone exposure intensity and duration in
China in 2015. Meteorological data, elevation data, emissions
inventories, land use data, vegetation indexes, road density data
and population density data were prepared based on 0.1°  0.1°
resolution to model the daily maximum 8-h mean ozone concen-
tration. The contribution of meteorological parameters was found
to be 65%, and the contribution of evaporation, which is a compre-
hensive index of temperature and humidity and has an important
influence on the formation and stability of ozone, was especially
notable. The authors also compared results with the spatiotempo-
ral kriging interpolation method, showing that the performance of
the random forest model was slightly higher (the R2 of the random
forest model was 0.69, while the R2 of the interpolation method
was 0.68).
3.3. Artificial neural network model
The artificial neural network is a nonlinear complex network
system composed of a large number of simple neurons. In the
learning process of the neural network, the connection and topol-
ogy of each neuron are constantly changing under the external
stimulus until the network output gradually approaches the
expected output. The model can be divided into a feedforward neu-
ral network and a feedback neural network. Convolutional neural
networks, as a type of deep feedforward neural network model,
reduce the complexity of network models, have the ability to per-
form hierarchical learning and can accurately extract features
(Chang, 2013; Lei, 2018).
Similar to the random forest model, the artificial neural net-
work has many advantages, but few studies implementing this
method are currently used for ground-level ozone simulation.
Di et al. (2017a) established a convolutional neural network
model that considered neighboring information through the
introduction of the convolutional layer and used remote sensing
ozone products, nitrogen oxide and sulfur dioxide data from
both monitoring sites and satellite-based products, volatile
organic compound (VOC) data from monitoring sites, chemical
transport model outputs, meteorological data and land use vari-
ables to simulate near-surface ozone exposure based on a
1 km  1 km grid in the United States from 2000 to 2012. R2
reached 0.76, which indicates good performance. These predic-
tive results were used in epidemiological studies that assessed
the relationship between ozone and mortality in the U.S. from
2000 to 2012 (Di et al., 2017b).
4. Discussion
We have reviewed the multiparameter statistical models used
to simulate high-resolution ground-level ozone exposure. This
review is of great significance for the development of future epi-
demiological studies and facilitates the use of accurate exposure
assessment methods for subsequent studies. Furthermore, this
review can provide a basic understanding from some perspectives
for the introduction of policies and management measures to pre-
vent and control the adverse effects of ambient ozone on human
health. We will introduce the basic process of developing research
that simulates ground-level ozone exposure using statistical mod-
els and compare the differences between studies to provide sug-
gestions for future studies.
 R. Ma et al. / Science of the Total Environment 701 (2020) 134463
4.1. Model selection
The most suitable model should be chosen after considering the
study purpose, study area, data availability, and computing
resources.
Currently, the LUR model is more widely used than the random
forest and artificial neural network models, and the reasons are
discussed as follows. First, the models have undergone long-term
development, and all aspects of the technology are mature, with
fewer types of parameters, simpler operations and higher spatial
resolutions. Furthermore, this model uses practical experience by
setting parameter weights to establish models, which can avoid
unreasonable results (Shi and Wang, 2016). However, it also has
disadvantages, such as unstable modeling methods and poor spa-
tial and temporal migration (Hoek et al., 2008). Different urban
structures may result in different model performances for the same
model. We found that the LUR model was more likely to be used in
regions instead of whole countries because it has difficulty forming
a prediction for long-term time series due to the search for high
resolution. The LUR model has difficulty capturing small spatial
changes in concentrations when the parameters of the study area
are not very variable. When the change is too large, the modeled
concentration tends to be higher than the true exposure, and the
correlation is poor (Briggs et al., 2000).
The random forest and neural network models are black-box
models that explore the relationship between ozone exposure
and different variables and realize the rapid calculation of large-
scale pollution simulations. The random forest model improves
performance without drastically increasing computational com-
plexity. In addition, it can obtain the order of parameter contribu-
tions, has high insensitivity to multivariate collinearity, and has
high stability with missing and unbalanced data; thus, it can
explain the influences of thousands of variables and does not need
to be normalized (Li, 2013). Furthermore, random forest models
have certain advantages that can help to avoid overfitting: a model
with more trees obtains a limited generalization error (Breiman,
2001; Shu, 2013). However, it is not easy to explain the results dur-
ing the process because of random forest models are black-box
models. The artificial neural network has excellent performance
and wide adaptability; however, it converges slowly and easily
overfits high-dimensional features, and a large number of calcula-
tions results are required by the research team, which burdens the
computing platform. The random forest model and artificial neural
network are more advantageous than the regression model when
handling multiparameter data, and they have prediction advan-
tages for long-term time series and large study sites.
After obtaining a good understanding of the basic research sit-
uation, including the study purpose and the advantages and disad-
vantages of different models, researchers can choose the
appropriate model according to their own needs. On this basis,
parameters can be collected and prepared.
4.2. Data preparation
4.2.1. Monitoring data
The research included in this review shows a very large differ-
ence in the area of the study region, from national scale to local
scale, which means that the number of monitoring sites varies
widely. Instead of routine monitoring networks, some investiga-
tors set passive samplers on purpose or select stations for special
design (Wolf et al., 2017; Malmqvist et al., 2014; Wang et al.,
2015, 2016; Kerckhoffs et al., 2015). Purpose-designed monitoring
sites normally consider population exposure. The researchers
divide the sites into categories, such as regional background, urban
background, traffic sites and industrial sites, or simply set monitor-
ing sites at the location of the subjects. Wang et al. (2015)
5
compared the difference between fixed sites and purpose-
designed samplers: the R2 value for fixed locations ranged from
0.65 to 0.88, while for the predictions at home sites, the R2 value
was between 0.60 and 0.91. Using purpose-designed monitoring
or multiple sources of monitoring data can improve the ability to
capture spatiotemporal variations in the model on a small scale,
but it cannot adapt to the requirements for conducting large-
scale studies.
In addition to differences in the number and type of monitoring
network, the length and continuity in the time series of the moni-
toring data are also different. The metric used in the model should
consider future applications. For health effects caused by long-
term exposure, complete time series are more important than high
temporal resolutions for the modeled results. For example, Wang
et al. (2015) simulated two-week, ground-level ozone exposure
from 1999 to 2013 in America. Due to the sample period, the
weekly time frame for the monitoring data limited the prediction
ability for 8-h maximum values that are commonly used, but
investigators believed that the two-week time scale can reduce
the impact of meteorological factors and time autocorrelation.
For studies focusing on acute health effects, high-temporal-
resolution metrics are needed. LUR models often fail to form
long-term time series in pursuit of a high spatial resolution, which
is one of the issues that researchers should consider when choos-
ing models. For studies that include long time scales and high res-
olutions, the machine-learning method is better.
4.2.2. Parameter selection and preparation
Multiparameters are a major feature used to simulate ambient
ozone concentrations based on statistical models. They can extend
the variable category and adjust the variable form. The explanatory
ability of the model can be improved, and the influences of specific
variables can be highlighted (Wu et al., 2016). The multiparameter
trend for ambient ozone simulation is definite. Thus, parameters
can be considered in several ways.
First, the mechanism of ground-level ozone formation should
be considered. Ground-level ozone is a typical secondary atmo-
spheric pollutant and is formed by a series of photochemical
reactions of nitrogen oxides (NOx) and VOCs under ultraviolet
light at a suitable temperature. A variety of typical factors
directly affect the formation of ground-level ozone, including
the concentration of precursor materials, meteorological factors,
and traffic-related factors affecting propagation. Socioeconomic,
land use, vegetation coverage and other factors also have a cer-
tain impact on the formation and diffusion of the ground-level
ozone concentration (Chen et al., 2017). More specifically, the
parameters can include 1) meteorological parameters such as
wind speed, wind direction, solar radiation, temperature, rainfall,
and relative humidity, 2) geographic variables such as land use
data, green space data, traffic data, residential and population
density data, regional indicators, elevation, 3) emissions inven-
tory parameters such as NO, NO2, organic carbon, NOx, VOCs,
SO2 and particulate matter, and 4) monitoring site parameters
such as NOx, sulfur oxides, VOCs and other pollutants at the
ground monitoring site. Data products reflecting the formation,
distribution and simulation of ground-level ozone concentra-
tions, such as satellite data products provided by open platforms,
such as the National Aeronautics and Space Administration
(NASA) and CTM products from previous studies, were also used
in models to improve performance.
Furthermore, after considering factors that influence the for-
mation of ground-level ozone, new researchers can be inspired
by previous researches on the contribution of parameters. The
contributions of variables vary by study. Zhan et al. (2018) found
that meteorological variables have the highest relative impor-
tance, accounting for 65%, with the highest contributions being
6 R. Ma et al. / Science of the Total Environment 701 (2020) 134463
attributed to evaporation, temperature and humidity. Son et al.
(2018) found that detailed emission patterns from local pollution
sources, coupled with wind field data (wind speed, wind direction
and boundary layer height), are needed to improve current LUR
models. Altitude (Beelen et al., 2009; Wang et al., 2016), road
density, residential land (Beelen et al., 2009), green space and
primary emission feature (traffic, population and impervious
surfaces) (Wang et al., 2016) data are also contributors. Further-
more, Wang et al. (2016) and De Hoogh et al. (2018) found that
the use of CTMs results in models with improved performance.
Some variable contributions were opposite in different studies.
For example, Wang et al. (2015) found that smaller-scale GIS
covariates, such as road network and population density, cannot
represent the characteristics of ambient ozone well, which may
lead to poor performance of the ozone simulation model. More
kinds of parameters can be involved in the model, and the appro-
priate parameters can be selected during the model development
process.
After parameter selection, the process of preparing key
parameters varied in previous articles. The specific metrics of
some variables were different based on data availability and
the aims of the investigators. Taking traffic data as an example,
a multicenter study conducted in Europe found that there was
no high-resolution European database for roads, and traffic flow
data were not consistently available in these countries; thus,
road length was the only traffic variable in the model (Beelen
et al., 2009). Some studies calculated conclusive variables to rep-
resent local traffic conditions, like traffic density. However, the
definition of traffic density is not the same in each study. Most
LUR studies considered traffic density to be a long-term variable
(Hoek et al., 2008). Adam-Poupart et al. (2014) defined traffic
density as kilometers of road within a circular area with a 1-
km radius, while Son et al. (2018) manually coded traffic density
from the Google traffic website, and Kerckhoffs et al. (2015) used
traffic counts multiplied by 48 to obtain traffic intensities during
daytime hours and then by 1.29 to calculate traffic intensities
per 24-hour period. Some studies used multiple variables instead
of conclusive variables, including road length, distance to nearby
major roads and, within buffers, lengths of roads and truck
routes and counts of intersections, to determine the specific rela-
tionship between traffic and ambient ozone (Wang et al., 2015).
The quality of the raw traffic data was variable. Wang et al.
(2015) used monitoring data from air quality system (AQS) mon-
itors, which were purposefully placed away from roads, and
studies using these data may have underestimated the effects
of traffic indicators. Researcher considerations also impact data
preparation. For example, Wolf et al. (2017) divided land use
data into residential, industrial, built-up, urban green, forest,
seminatural and water body areas, while Malmqvist et al.
(2014) defined land use data as high-density residential, low-
density residential, industrial, port, urban green, seminatural
and forested areas. Four types of land use data were defined
by Huang et al. (2017), including residential land, agricultural
land, green spaces and water bodies.
The selection process mainly depends on the formation mecha-
nism of ambient ozone and previous studies or experience. Param-
eters commonly used in the model mainly include 1)
meteorological variables such as temperature, humidity, evapora-
tion, solar radiation, wind speed, boundary layer height, and pre-
cipitation, 2) precursor concentration, 3) geographical variables
such as land use term, vegetation cover, and elevation, 4) emission
inventory, 5) socioeconomic factors such as transportation, resi-
dential and population density, and 6) simulation products such
as chemical transport model output (Table 1). Researchers can
change the definitions of specific parameters based on their aims
to obtain an optimal combination.
4.3. Simulation scale determination
Due to the characteristics of data availability and study pur-
poses, the time-scale simulation can be divided into continuous
simulations and simulations for specific periods. Furthermore,
the spatial and temporal resolutions can be divided into high and
low resolutions. The high-spatiotemporal-resolution results can
provide fine-concentration population exposure, which can
improve accuracy and reduce conflicting factors, especially for
studies focusing on acute health effects. However, this also
increases the difficulty of data acquisition and processing and pre-
sents higher requirements for the hardware and software facilities
of the research team. The low-spatiotemporal-resolution results
can save time and manpower and obtain results more quickly.
For long-term exposure studies that have low requirements for
time-resolution results, researchers can choose metrics at the
annual or monthly level to improve effectiveness.
Based on study purpose and need, the model type can be cho-
sen. For finer simulations, especially on a large study scale with
complex trends, machine-learning methods performance better
than the LUR model. Although studies that focused on ambient
ozone exposure were rare, applications for other air pollutants
proved superior in some contexts. Using PM2.5 as an example, Hu
et al. (2017) used a random forest model in the United States in
2001 and obtained a simulation result of R2 = 0.8 based on a reso-
lution of 1 km  1 km; Zhan et al. (2017) used a geographically
weighted gradient lifting tree in China in 2014, and the result
was obtained based on a spatial resolution of 0.5°0.5°
(R2 = 0.76). Di et al. (2016) used a convolutional neural network
from 2000 to 2012 at a 1 km  1 km resolution and obtained a total
R2 of 0.84; Li et al. (2017) used a neural network in China in 2015,
with an R2 up to 0.88 based on a resolution of 0.1°0.1°.
4.4. Model development and validation
The process of model development varies based on model type.
The land use model builds a linear regression model using a series
of related variables to simulate ozone exposure. The random forest
model can be regarded as a regression model when simulating
ozone concentration by building relationships between indepen-
dent and dependent variables. The neural network freely learns
any function form from the training data to simulate the ozone
concentration. Di et al. (2017a) considered neighboring informa-
tion during the modeling process through the introduction of a
convolutional layer.
The processes of developing models based on regression algo-
rithms and machine-learning algorithms are similar: model
parameters and features are constantly adjusted to achieve opti-
mal performance. Regression algorithms and machine-learning
algorithms have similarities and differences in terms of model
establishment and verification.
However, the development processes of the three models could
be different. For the LUR model, parameter selection, which is
mainly conducted through a supervised stepwise procedure, is
important. Basically, a regression model is used for all potential
predictors and the one with the highest explained variance is cho-
sen. Then, researchers add further predictors step by step if the
increase in adjusted R2 is >1%. Some researchers use a priori effect
direction for each variable and require that the effect direction of
the variable included must be the same as the a priori direction
and that the effect direction of variables already in the model does
not change. According to these researchers, not constraining a pri-
ori directions leads to models that make unrealistic predictions. A
constraint was needed because there was considerable collinearity
between predictor variables (Beelen et al., 2009). Others had the
opposite view: ozone, as a secondary pollutant, was involved in
 R. Ma et al. / Science of the Total Environment 701 (2020) 134463
many reactions, and the effect directions were unclear (Malmqvist
et al., 2014). Other researchers (Son et al., 2018) used the least
absolute shrinkage and selection operator (LASSO) method, which
aims to improve the prediction accuracy and interpretability of the
model (Tibshirani, 1996) and the performance of the traditional
LUR method. Developing a multivariate logistic regression model
requires knowing the optimal number of prognostic factors to
include. The LASSO method has a smaller mean square error
(MSE) than conventional methods and handles the multicollinear-
ity problem. Some researchers defined their own methods; for
example, Wang et al (2015) developed a hierarchical spatiotempo-
ral model to accommodate unique features and selected the best
model based on the cross-validated R2 value. Furthermore, restric-
tions were proposed to remove variables in some situations. These
restrictions aimed to improve the stability of the models (Wolf
et al., 2017; Wang et al., 2015). For example, Wolf et al. set the fol-
lowing conditions: at least five sites must exhibit different values
and the minimum or maximum values must lie within threefold
of the 10th to 90th percentile range below or above the 10th and
90th percentiles. In this way, the selection of specific predictors
that included mainly zeros or extreme outliers was prevented.
For the machine-learning method, like the integrated learning
algorithm, parameter selection is mainly achieved by performing
subsequent operations based on model importance ordering of
all parameters. The important parameters were number of vari-
ables included in every tree and the number of trees. Meanwhile,
the deep learning algorithm has the ability to automatically learn
features. The hidden layer number, hidden node number and active
function should be set. These model parameters should be adjusted
during the model development process depending on model per-
formance, mainly reflecting R2, R, MSE, and RMSE, which are calcu-
lated during the validation process.
The main validation method is the cross-validation (CV)
method, which can be divided into two types in these articles.
The first type is leave-out-one cross validation (Wolf et al., 2017),
which is the most common CV method (Geisser, 1974). In this field,
the basic idea is that a monitoring station is excluded from the
total number of sampling sites (K) to generate training datasets
with K-1 sites, resulting in fitted models that simulate pollutant
concentrations at the excluded sites (test set). This method is com-
monly used for the LUR model and has been criticized for overes-
timating predictive ability (Wang et al., 2013). The other method
is V-fold CV (Son et al., 2018), where V = 10, which means that
the monitoring data are divided into 10 random splits, 9 for train-
ing the model and 1 for testing the model performance, until the
best model performance is achieved, is the most common (Wang
et al., 2015). Some researchers set the cut-off values at 75% and
25% (Beelen et al., 2009) or 80% and 20% (De Hoogh et al., 2018).
In addition to model performance, the set of model parameters
is also limited by the computing resources; for example, a higher
tree number and number of steps for iteration would lead to better
model performance in some contexts but also to a longer calcula-
tion time. The research team can set the parameters according to
research purpose and ability and finally establish the optimal
model at the current level.
4.5. Application of the simulation results
A few studies modeled ground-level ozone exposure in Europe,
North America and China, and some results have been used in epi-
demiological studies (Holle et al., 2005; Yang et al., 2018). The high
resolution of modeled ambient ozone exposure data provided a
chance, in some contexts, to effectively explore the relationship
between ozone and human health.
Some studies achieved high model performance, but the robust-
ness of the studies, i.e., what might happen when the model is
7
extrapolated to other regions, should be considered. Some studies
have found factors that influence the robustness of the models. The
degree of urbanization and the distribution of the monitoring sites
vary by region, so care should be taken when the data are extrap-
olated to other regions. For example, Wang et al. (2015) noted that
models are limited when applied to areas where monitoring net-
works were sparse; Adam-Poupart et al. (2014) found that esti-
mates exhibit higher discrepancies from data values that are
mostly from regions characterized by data scarcity. Kerckhoffs
et al. (2015) found that, by excluding some observations, which
increased the urbanization of sites, the robustness of the model
remained good. Furthermore, Beelen et al. (2009) found that
extrapolating far beyond the range of measured concentrations
would lead to errors, with a possible solution being truncating
the predicted concentrations to the highest measured concentra-
tion. To explore the relationship between ambient ozone and
health more precisely, more high-resolution exposure assessments
are needed, and care should be taken when assessment results are
extrapolated from other places.
4.6. Prospects and limitations
With the development of epidemiological studies, further stud-
ies are needed that focus on simulating ozone with high spatial and
temporal resolutions. Complete time series and large coverage
areas also provide convenience for the exposure assessments of
populations on a fine scale. On one hand, the daily modeling data
complemented the time series, especially provided historical expo-
sure data; on the other hand, the high-spatial-resolution modeling
results provide exposure data for areas without monitoring sites.
Exposure data at high spatial and temporal resolutions improves
exposure accuracy and reduces possible exposure assessment
errors for both acute and chronic environmental epidemiological
studies. The modeling results are derived from statistical models
based on a variety of parameters affecting ozone formation and
elimination. The errors caused by relying solely on ozone monitor-
ing instruments are reduced, as well as the errors due to the lim-
ited number and placement of monitoring stations. Furthermore,
the modeling results with high spatial and temporal resolutions
can better represent the spatiotemporal variability in the ambient
ozone distribution and reduce the exposure error. Compared with
developed countries, developing countries with shorter monitoring
histories and rare distributions of monitoring air pollution stations
have greater demand for these studies. Furthermore, considering
the variance caused by the form of varied variables and the difficul-
ties in comparing results, standard databases that are capable of
multiple parameter requirements and shared platforms for
researchers are inevitable.
Limitations still exist in this field. First, current studies that
have focused on fine ambient ozone exposure modeling are limited
and need to be continuously developed. Most studies have focused
on low-pollution areas in developed countries, while few research-
ers have paid attention to highly polluted areas in developing
countries, where monitoring stations are sparsely distributed and
the monitoring history is not long. The demand for the fine-
resolution assessment from epidemiological studies has not been
completely met. Second, the validation of the modeling results
remains a limitation. Availability and effectiveness should be
tested not only by the model performance but also by the results
of epidemiological studies that use modeling results as exposure
data. Few studies have evaluated error type and the amount of
measurement error by comparing difference between true expo-
sure and simulated exposure using different exposure data, which
will affect health risk estimates and statistical power (Goldman
et al., 2011, 2012), and validation of modeling results was rarely
tested in environmental epidemiology. A joint indicator system
8 R. Ma et al. / Science of the Total Environment 701 (2020) 134463
should be established to assess the applicability of exposure and
provide a theoretical basis for use in environmental epidemiology.
5. Conclusion
Multiparameter statistical models have been used to simulate
ambient ozone exposure, which improves the accuracy of exposure
assessment in epidemiological studies. This review summarized
the basic process of model development in terms of model selec-
tion, data preparation, determination of simulation scale, and
model development and validation, introducing the underlying
context and method for whole processes. Land use regression mod-
els are mature modeling techniques with low computational com-
plexity, and they are easy to use to obtain satisfying model
performance at small scales; however, they have limited capacities
to capture temporal variations and can miss short-term and regio-
nal patterns. Comparatively, machine-learning algorithms are bet-
ter at processing multiparameter data in larger research areas,
which increases computational requirements. The models have
their own characteristics, and the study purpose, study area, data
availability, and computing resources should be considered during
the model selection and development process. In the future, fur-
ther research based on multiple parameters and different simula-
tion scales is needed.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgments
This work was funded by grants from the National Key Research
and Development Program of China (Grant: 2017YFC0211706), the
Special Foundation of Basic Science and Technology Resources Sur-
vey of the Ministry of Science and Technology of China (Grant:
2017FY101204), and the Beijing Natural Science Foundation
(7172145).
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