Health burden from food systems is highly unequal across income groups.

Food consumption contributes to the degradation of air quality in regions where food is produced, creating a contrast between the health burden caused by a specific population through its food consumption and that faced by this same population as a consequence of food production activities. Here we explore this inequality within China's food system by linking air-pollution-related health burden from production to consumption, at high levels of spatial and sectorial granularity. We find that low-income groups bear a 70% higher air-pollution-related health burden from food production than from food consumption, while high-income groups benefit from a 29% lower health burden relative to their food consumption. This discrepancy largely stems from a concentration of low-income residents in food production areas, exposed to higher emissions from agriculture. Comprehensive interventions targeting both production and consumption sides can effectively reduce health damages and concurrently mitigate associated inequalities, while singular interventions exhibit limited efficacy.

Increased air pollution exposure among the Chinese population during the national quarantine in 2020.

The COVID-19 quarantine in China is thought to have reduced ambient air pollution. The overall exposure of the population also depends, however, on indoor air quality and human mobility and activities. Here, by integrating real-time mobility data and a questionnaire survey on time-activity patterns during the pandemic, we show that despite a decrease in ambient PM2.5 during the quarantine, the total population-weighted exposure to PM2.5 considering both indoor and outdoor environments increased by 5.7 µg m-3 (95% confidence interval, 1.2-11.0 µg m-3). The increase in population-weighted exposure was mainly driven by a nationwide urban-to-rural population migration before the Spring Festival coupled with the freezing of the migration backward due to the quarantine, which increased household energy consumption and the fraction of people exposed to rural household air pollution indoors. Our analysis reveals an increased inequality of air pollution exposure during the quarantine and highlights the importance of household air pollution for population health in China.

A multiphase CMAQ version 5.0 adjoint.

We present the development of a multiphase adjoint for the Community Multiscale Air Quality (CMAQ) model, a widely used chemical transport model. The adjoint model provides location- and time-specific gradients that can be used in various applications such as backward sensitivity analysis, source attribution, optimal pollution control, data assimilation, and inverse modeling. The science processes of the CMAQ model include gas-phase chemistry, aerosol dynamics and thermodynamics, cloud chemistry and dynamics, diffusion, and advection. Discrete adjoints are implemented for all the science processes, with an additional continuous adjoint for advection. The development of discrete adjoints is assisted with algorithmic differentiation (AD) tools. Particularly, the Kinetic PreProcessor (KPP) is implemented for gas-phase and aqueous chemistry, and two different automatic differentiation tools are used for other processes such as clouds, aerosols, diffusion, and advection. The continuous adjoint of advection is developed manually. For adjoint validation, the brute-force or finite-difference method (FDM) is implemented process by process with box- or column-model simulations. Due to the inherent limitations of the FDM caused by numerical round-off errors, the complex variable method (CVM) is adopted where necessary. The adjoint model often shows better agreement with the CVM than with the FDM. The adjoints of all science processes compare favorably with the FDM and CVM. In an example application of the full multiphase adjoint model, we provide the first estimates of how emissions of particulate matter (PM2.5) affect public health across the US.

Simulation of airborne trace metals in fine particulate matter over North America.

Trace metal distributions are of relevance to understand sources of fine particulate matter (PM2.5), PM2.5-related health effects, and atmospheric chemistry. However, knowledge of trace metal distributions is lacking due to limited ground-based measurements and model simulations. This study develops a simulation of 12 trace metal concentrations (Si, Ca, Al, Fe, Ti, Mn, K, Mg, As, Cd, Ni and Pb) over continental North America for 2013 using the GEOS-Chem chemical transport model. Evaluation of modeled trace metal concentrations with observations indicates a spatial consistency within a factor of 2, an improvement over previous studies that were within a factor of 3-6. The spatial distribution of trace metal concentrations reflects their primary emission sources. Crustal element (Si, Ca, Al, Fe, Ti, Mn, K) concentrations are enhanced over the central US from anthropogenic fugitive dust and over the southwestern U.S. due to natural mineral dust. Heavy metal (As, Cd, Ni and Pb) concentrations are high over the eastern U.S. from industry. K is abundance in the southeast from biomass burning and high concentrations of Mg is observed along the coast from sea spray. The spatial pattern of PM2.5 mass is most strongly correlated with Pb, Ni, As and K due to their signature emission sources. Challenges remain in accurately simulating observed trace metal concentrations. Halving anthropogenic fugitive dust emissions in the 2011 National Air Toxic Assessment (NATA) inventory and doubling natural dust emissions in the default GEOS-Chem simulation was necessary to reduce biases in crustal element concentrations. A fivefold increase of anthropogenic emissions of As and Pb was necessary in the NATA inventory to reduce the national-scale bias versus observations by more than 80 %, potentially reflecting missing sources.

A Call for an Aloft Air Quality Monitoring Network: Need, Feasibility, and Potential Value.

Changing precursor emission patterns in conjunction with stringent health protective air quality standards necessitate accurate quantification of nonlocal contributions to ozone pollution at a location due to atmospheric transport, that by nature predominantly occurs aloft nocturnally. Concerted efforts to characterize ozone aloft on a continuous basis to quantify its contribution to ground-level concentrations, however, are lacking. By applying our classical understanding of air pollution dynamics to analyze variations in widespread surface-level ozone measurements, in conjunction with process-based interpretation from a comprehensive air pollution modeling system and detailed backward-sensitivity calculations that quantitatively link surface-level and aloft pollution, we show that accurate quantification of the amount of ozone in the air entrained from aloft every morning as the atmospheric boundary layer grows is the key missing component for characterizing background pollution at a location, and we propose a cost-effective continuous aloft ozone measurement strategy to address critical scientific gaps in current air quality management. Continuous aloft air pollution measurements can be achieved cost-effectively through leveraging advances in sensor technology and proliferation of tall telecommunications masts. Resultant improvements in ozone distribution characterization at 400-500 m altitude are estimated to be 3-4 times more effective in characterizing the surface-level daily maximum 8-h average ozone (DM8O3) than improvements from surface measurements since they directly quantify the amount of pollution imported to a location and furnish key missing information on processes and sources regulating background ozone and its modulation of ground-level concentrations. Since >80% of the DM8O3 sensitivity to tropospheric ozone is potentially captured through measurements between 200 and 1200 m altitude (a possible design goal for future remote sensing instrumentation), their assimilation will dramatically improve air quality forecast and health advisories.

Diminishing Returns or Compounding Benefits of Air Pollution Control? The Case of NOx and Ozone.

UNLABELLED: A common measure used in air quality benefit-cost assessment is marginal benefit (MB), or the monetized societal benefit of reducing 1 ton of emissions. Traditional depictions of MB for criteria air pollutants are such that each additional ton of emission reduction incurs less benefit than the previous ton. Using adjoint sensitivity analysis in a state-of-the-art air quality model, we estimate MBs for NOx emitted from mobile and point sources, characterized based on the estimated ozone-related premature mortality in the U.S. POPULATION: Our findings indicate that nation-wide emission reductions in the U.S. significantly increase NOx MBs for all sources, without exception. We estimate that MBs for NOx emitted from mobile sources increase by 1.5 and 2.5 times, on average, for 40% and 80% reductions in anthropogenic emissions across the U.S. Our results indicate a strictly concave damage function and compounding benefits of progressively lower levels of NOx emissions, providing economic incentive for higher levels of abatement than were previously advisible. These findings suggest that the traditional perception of a convex damage function and decreasing MB with abatement may not hold true for secondary pollutants such as O3.

Optimal Ozone Control with Inclusion of Spatiotemporal Marginal Damages and Electricity Demand.

Marginal damage (MD), or damage per ton of emission, is a policy metric used for effective pollution control and reducing the corresponding adverse health impacts. However, for a pollutant such as NOx, the MD varies by the time and location of the emissions, a complication that is not adequately accounted for in the currently implemented economic instruments. Policies accounting for MD information would aim to encourage emitters with large MDs to reduce their emissions. An optimization framework is implemented to account for NOx spatiotemporal MDs calculated through adjoint sensitivity analysis and to simulate power plants' behavior under emission and simplified electricity constraints. The results from a case study of U.S. power plants indicate that time-specific MDs are high around noon and low in the evening. Furthermore, an emissions reduction of about 40% and a net benefit of about $1200 million can be gained for this subset of power plants if a larger fraction of the electricity demand is supplied by power plants at low-damage times and in low-damage locations. The results also indicate that the consideration of temporal effects in NOx control policies results in a comparable net benefit to the consideration of spatial or spatiotemporal effects, thus providing a promising option for policy development.

Differences between magnitudes and health impacts of BC emissions across the United States using 12 km scale seasonal source apportionment.

Recent assessments have analyzed the health impacts of PM2.5 from emissions from different locations and sectors using simplified or reduced-form air quality models. Here we present an alternative approach using the adjoint of the Community Multiscale Air Quality (CMAQ) model, which provides source-receptor relationships at highly resolved sectoral, spatial, and temporal scales. While damage resulting from anthropogenic emissions of BC is strongly correlated with population and premature death, we found little correlation between damage and emission magnitude, suggesting that controls on the largest emissions may not be the most efficient means of reducing damage resulting from anthropogenic BC emissions. Rather, the best proxy for locations with damaging BC emissions is locations where premature deaths occur. Onroad diesel and nonroad vehicle emissions are the largest contributors to premature deaths attributed to exposure to BC, while onroad gasoline emissions cause the highest deaths per amount emitted. Emissions in fall and winter contribute to more premature deaths (and more per amount emitted) than emissions in spring and summer. Overall, these results show the value of the high-resolution source attribution for determining the locations, seasons, and sectors for which BC emission controls have the most effective health benefits.

Attainment vs exposure: ozone metric responses to source-specific NOx controls using adjoint sensitivity analysis.

We establish linkages between sources of NOx emissions and two types of national ozone metrics in Canada and the U.S. using the adjoint of an air quality model. We define an attainment-based metric using probabilistic design values (PDVs) exceeding 65 ppb to represent polluted regions and define an exposure-based metric as the premature mortality count related to short-term ozone exposure, both in Canada and the U.S. Our results reveal differences in both temporally averaged and day-specific influences of NOx emission controls across source locations. We find NOx emission reductions in California and the eastern U.S. to be most effective for reducing attainment- and exposure-based metrics, amounting to a total reduction of 6500 ppb in PDVs and 613 deaths/season nationally from a 10% reduction in NOx emissions from those source locations. While source controls in the remainder of the western U.S. are beneficial at reducing nonattainment, these reductions are less influential on ozone mortality. We also find that while exposure-based metrics are sensitive to daily emission reductions, much of the reduction in PDVs arises from controlling emissions on only a fraction of simulation days. We further illustrate the dependency of adjoint estimates of emission influences on the choice of averaging period as a follow-up to previous work.

Optimal ozone reduction policy design using adjoint-based NOx marginal damage information.

Despite substantial reductions in nitrogen oxide (NOx) emissions in the United States, the success of emission control programs in optimal ozone reduction is disputable because they do not consider the spatial and temporal differences in health and environmental damages caused by NOx emissions. This shortcoming in the current U.S. NOx control policy is explored, and various methodologies for identifying optimal NOx emission control strategies are evaluated. The proposed approach combines an optimization platform with an adjoint (or backward) sensitivity analysis model and is able to examine the environmental performance of the current cap-and-trade policy and two damage-based emissions-differentiated policies. Using the proposed methodology, a 2007 case study of 218 U.S. electricity generation units participating in the NOx trading program is examined. The results indicate that inclusion of damage information can significantly enhance public health performance of an economic instrument. The net benefit under the policy that minimizes the social cost (i.e., health costs plus abatement costs) is six times larger than that of an exchange rate cap-and-trade policy.

Source attribution of health benefits from air pollution abatement in Canada and the United States: an adjoint sensitivity analysis.

BACKGROUND: Decision making regarding air pollution can be better informed if air quality impacts are traced back to individual emission sources. Adjoint or backward sensitivity analysis is a modeling tool that can achieve this goal by allowing for quantification of how emissions from sources in different locations influence human health metrics. OBJECTIVES: We attributed short-term mortality (valuated as an overall "health benefit") in Canada and the United States to anthropogenic nitrogen oxides (NO(x)) and volatile organic compound (VOC) emissions across North America. METHODS: We integrated epidemiological data derived from Canadian and U.S. time-series studies with the adjoint of an air quality model and also estimated influences of anthropogenic emissions at each location on nationwide health benefits. RESULTS: We found significant spatiotemporal variability in estimated health benefit influences of NO(x) and VOC emission reductions on Canada and U.S. mortality. The largest estimated influences on Canada (up to $250,000/day) were from emissions originating in the Quebec City-Windsor Corridor, where population centers are concentrated. Estimated influences on the United States tend to be widespread and more substantial owing to both larger emissions and larger populations. The health benefit influences calculated using 24-hr average ozone (O(3)) concentrations are lower in magnitude than estimates calculated using daily 1-hr maximum O(3) concentrations. CONCLUSIONS: Source specificity of the adjoint approach provides valuable information for guiding air quality decision making. Adjoint results suggest that the health benefits of reducing NO(x) and VOC emissions are substantial and highly variable across North America.

Improving NO(x) cap-and-trade system with adjoint-based emission exchange rates.

Cap-and-trade programs have proven to be effective instruments for achieving environmental goals while incurring minimum cost. The nature of the pollutant, however, affects the design of these programs. NO(x), an ozone precursor, is a nonuniformly mixed pollutant with a short atmospheric lifetime. NO(x) cap-and-trade programs in the U.S. are successful in reducing total NO(x) emissions but may result in suboptimal environmental performance because location-specific ozone formation potentials are neglected. In this paper, the current NO(x) cap-and-trade system is contrasted to a hypothetical NO(x) trading policy with sensitivity-based exchange rates. Location-specific exchange rates, calculated through adjoint sensitivity analysis, are combined with constrained optimization for prediction of NO(x) emissions trading behavior and post-trade ozone concentrations. The current and proposed policies are examined in a case study for 218 coal-fired power plants that participated in the NO(x) Budget Trading Program in 2007. We find that better environmental performance at negligibly higher system-wide abatement cost can be achieved through inclusion of emission exchange rates. Exposure-based exchange rates result in better environmental performance than those based on concentrations.

The adjoint of CMAQ.

An adjoint model for the internationally used Community Multiscale Air Quality (CMAQ) modeling platform of the U.S. EPA is developed. The adjoint version for CMAQ (CMAQ-ADJ) provides the user community with forward (decoupled direct method or DDM) and backward (adjoint) sensitivity analysis capabilities. Current implementation is for gas-phase processes. Discrete adjoints are implemented for all processes with the exception of horizontal advection, for which, because of inherent discontinuities in the advection scheme, the continuous approach is superior. The adjoint of chemistry is constructed by interfacing CMAQ with the kinetic pre-processor, which provides for increased flexibility in the choice of chemical solver and facilitates the implementation of new chemical mechanisms. The adjoint implementation is evaluated both on a process-by-process basis and for the full model. In general, adjoint results show good agreement with brute-force and DDM sensitivities. As expected for a continuous adjoint implementation in a nonlinear scheme, the agreement is not perfect for horizontal transport. Sensitivities of various air quality, public health, and environmental metrics with respect to emissions are calculated using the adjoint method. In order to show applicability to regional climate studies, as an example, the sensitivities of these metrics with respect to local temperatures are calculated.

Adjoint sensitivity analysis of ozone nonattainment over the continental United States.

An application of the adjoint method in air quality management is demonstrated. We use a continental scale chemical transport model (STEM) to calculate the sensitivities of a nationwide U.S. ozone national ambient air quality standard (NAAQS) nonattainment metric to precursor emissions for the period July 1 to August 15, 2004. The model shows low bias and error (-4 and 24%, respectively), particularly for areas with high ozone concentrations. The nonattainment metric accounts for both 1-h and 8-h ozone standards, but is dominated by the 8-h exceedances (97% of the combined metric). Largest values of sensitivities are found to be with respect to emissions in the south and southeast U.S., Ohio River Valley, and California. When nonattainment sensitivities are integrated over the entire U.S., NOx emissions account for the largest contribution (62% of the total), followed by biogenic and anthropogenic VOCs (24% and 14%, respectively). For NOx emissions, point/area and mobile sources account for 54% and 46% of the total sensitivities, respectively. We also provide a state-by-state comparison for the nonattainment magnitude, nonattainment sensitivity, and emission magnitudes to explore the influence of interstate transport of ozone and its precursors, and policy implications of the results. Our analysis of the nationwide ozone nonattainment metric suggests that simple cap-and-trade programs may prove inadequate in achieving sought-after air quality objectives.

Nonlinear response of ozone to emissions: source apportionment and sensitivity analysis.

For secondary air pollutants, precursor emissions may impact concentrations in nonlinear and interdependent manners. We explore the nonlinear responses of one such pollutant, ozone, to emissions of its precursors, nitrogen oxides (NOx) and volatile organic compounds. Modeling is conducted for a high ozone episode in the southeastern United States, applying a second-order direct sensitivity method in a regional air quality model. As applied here, the sensitivity method neglects most aerosol and aqueous chemistry processes. Inclusion of second-order sensitivities is shown to enable accurate characterization of response to large perturbations in emissions. An index is introduced to characterize the nonlinearity of ozone response to NOx emitted from each source region. Nonlinearity is found to increase with the tonnage and emission density of the source region. Interactions among the impacts of emission sources are shown to lead to discrepancies between source contribution attributed to an ensemble of emitters and the sum of the contributions attributed to each component. A method is introduced for applying these "cross-sensitivity" interactions to assess the uncertainty of sensitivity and source apportionment estimates arising from uncertainty in an emissions inventory. For ozone response to NOx, underestimates in emission rates lead to underprediction of total source contribution but overprediction of per-ton sensitivity.

Ozone formation potential of organic compounds in the Eastern United States: a comparison of episodes, inventories, and domains.

Direct sensitivity analysis is applied for 3-D assessment of ozone reactivity (or ozone formation potential) in the Eastern United States. A detailed chemical mechanism (SAPRC-99) is implemented in a multiscale air quality model to calculate the reactivity of 32 explicit and 9 lumped compounds. Simulations are carried out for two different episodes and two different emission scenarios. While absolute reactivities of VOCs show a great deal of spatial variability, relative reactivities (normalized to the reactivity of a base mixture) produce a significantly more homogeneous field. Three types of domain-wide relative reactivity metrics are formed for 1-h and 8-h averaging intervals. In general, ozone reactivity metrics (with the exception of those based on daily peak ozone) are fairly robust and consistent between different episodes or emission scenarios. The 3-D metrics also show fairly similar rankings for VOC reactivity when compared to the box model scales. However, the 3-D metrics have a noticeably narrower range for species reactivities, as they result in lower reactivity for some of the more reactive, radical-producing VOCs (especially aldehydes). As expected, episodes and emission scenarios with less radical availability have higher absolute reactivities for all species and higher relative reactivities for the more radical-producing species. Finally, comparing the results with those from a different domain (central California) shows that relative reactivity metrics are comparable over these two significantly different domains.

High-order, direct sensitivity analysis of multidimensional air quality models.

A direct sensitivity analysis technique is extended to calculate higher-order sensitivity coefficients in three-dimensional air quality models. The time evolution of sensitivity coefficients of different order is followed alongside that of the concentrations. Calculation of higher-order sensitivity coefficients requires few modifications to the original (first-order) sensitivity modules and is carried out efficiently and with minimal computational overhead. The modeling results (first-, second-, and third-order sensitivity coefficients) for an ozone episode in central California are shown and discussed. Second-order sensitivity coefficients of ozone concentration with respect to domain-wide NO emissions show reasonable agreement with brute-force results and exhibit less noisy behavior. By using second-order sensitivity coefficients the nonlinear responses are better captured and described. For a Taylor series projection from the base case, including the second-order term improves the accuracy. In general, higher-order sensitivity analysis shows a noticeable improvement in terms of accuracy over the conventional first-order analysis. Of particular interest, second-order sensitivity analysis is better equipped to address the nonlinear behavior around the peak ozone in NO(x)-rich plumes.