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  1. Abstract. Changes in anthropogenic aerosol emissions have strongly contributed to global and regional trends in temperature, precipitation, and other climate characteristics and have been one of the dominant drivers of decadal trends in Asian and African precipitation. These and other influences on regional climate from changes in aerosol emissions are expected to continue and potentially strengthen in the coming decades. However, a combination of large uncertainties in emission pathways, radiative forcing, and the dynamical response to forcing makes anthropogenic aerosol a key factor in the spread of near-term climate projections, particularly on regional scales, and therefore an important one to constrain. For example, in terms of future emission pathways, the uncertainty in future global aerosol and precursor gas emissions by 2050 is as large as the total increase in emissions since 1850. In terms of aerosol effective radiative forcing, which remains the largest source of uncertainty in future climate change projections, CMIP6 models span a factor of 5, from −0.3 to −1.5 W m−2. Both of these sources of uncertainty are exacerbated on regional scales. The Regional Aerosol Model Intercomparison Project (RAMIP) will deliver experiments designed to quantify the role of regional aerosol emissions changes in near-term projections. This is unlike any prior MIP, where the focus has been on changes in global emissions and/or very idealised aerosol experiments. Perturbing regional emissions makes RAMIP novel from a scientific standpoint and links the intended analyses more directly to mitigation and adaptation policy issues. From a science perspective, there is limited information on how realistic regional aerosol emissions impact local as well as remote climate conditions. Here, RAMIP will enable an evaluation of the full range of potential influences of realistic and regionally varied aerosol emission changes on near-future climate. From the policy perspective, RAMIP addresses the burning question of how local and remote decisions affecting emissions of aerosols influence climate change in any given region. Here, RAMIP will provide the information needed to make direct links between regional climate policies and regional climate change. RAMIP experiments are designed to explore sensitivities to aerosol type and location and provide improved constraints on uncertainties driven by aerosol radiative forcing and the dynamical response to aerosol changes. The core experiments will assess the effects of differences in future global and regional (Africa and the Middle East, East Asia, North America and Europe, and South Asia) aerosol emission trajectories through 2051, while optional experiments will test the nonlinear effects of varying emission locations and aerosol types along this future trajectory. All experiments are based on the shared socioeconomic pathways and are intended to be performed with 6th Climate Model Intercomparison Project (CMIP6) generation models, initialised from the CMIP6 historical experiments, to facilitate comparisons with existing projections. Requested outputs will enable the analysis of the role of aerosol in near-future changes in, for example, temperature and precipitation means and extremes, storms, and air quality.

     
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  2. Abstract

    Ascorbic acid is among the most abundant antioxidants in the lung, where it likely plays a key role in the mechanism by which particulate air pollution initiates a biological response. Because ascorbic acid is a highly redox active species, it engages in a far more complex web of reactions than a typical organic molecule, reacting with oxidants such as the hydroxyl radical as well as redox-active transition metals such as iron and copper. The literature provides a solid outline for this chemistry, but there are large disagreements about mechanisms, stoichiometries and reaction rates, particularly for the transition metal reactions. Here we synthesize the literature, develop a chemical kinetics model, and use seven sets of laboratory measurements to constrain mechanisms for the iron and copper reactions and derive key rate constants. We find that micromolar concentrations of iron(III) and copper(II) are more important sinks for ascorbic acid (both AH2and AH) than reactive oxygen species. The iron and copper reactions are catalytic rather than redox reactions, and have unit stoichiometries: Fe(III)/Cu(II) + AH2/AH + O2→ Fe(III)/Cu(II) + H2O2 + products. Rate constants are 5.7 × 104and 4.7 × 104 M−2 s−1for Fe(III) + AH2/AHand 7.7 × 104and 2.8 × 106 M−2 s−1for Cu(II) + AH2/AH, respectively.

     
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