Reactive atmospheric halogens destroy tropospheric ozone (O 3), an air pollutant and greenhouse gas. The primary source of natural halogens is emissions from marine phytoplankton and algae, as well as abiotic sources from ocean and tropospheric chemistry, but how their fluxes will change under climate warming-and the resulting impacts on O 3-are not well known. Here we use an Earth system model to estimate that natural halogens deplete approximately 13 % of tropospheric O 3 in the presentday climate. Despite increased levels of natural halogens through the twenty-first century, this fraction remains stable due to compensation from hemispheric, regional, and vertical heterogeneity in tropospheric O 3 loss. Notably, this halogen-driven O 3 buffering is projected to be greatest over polluted and populated regions, mainly due to iodine chemistry, with important implications for air quality. Tropospheric O 3 is a trace gas that plays a key role in atmospheric chemistry, both as a greenhouse gas and as a component of photochemical smog, affecting air quality and public health. 1,2 Its abundance is controlled by a balance between in-situ Glob. Environ. Chang. 42, 346-358 (2017).
Arctic feedbacks accelerate climate change through carbon releases from thawing permafrost and higher solar absorption from reductions in the surface albedo, following loss of sea ice and land snow. Here, we include dynamic emulators of complex physical models in the integrated assessment model PAGE-ICE to explore nonlinear transitions in the Arctic feedbacks and their subsequent impacts on the global climate and economy under the Paris Agreement scenarios. The permafrost feedback is increasingly positive in warmer climates, while the albedo feedback weakens as the ice and snow melt. Combined, these two factors lead to significant increases in the mean discounted economic effect of climate change: +4.0% ($24.8 trillion) under the 1.5 °C scenario, +5.5% ($33.8 trillion) under the 2 °C scenario, and +4.8% ($66.9 trillion) under mitigation levels consistent with the current national pledges. Considering the nonlinear Arctic feedbacks makes the 1.5 °C target marginally more economically attractive than the 2 °C target, although both are statistically equivalent.
CH4 is the most abundant reactive greenhouse gas and a complete understanding of its atmospheric fate is needed to formulate mitigation policies. Current chemistry-climate models tend to underestimate the lifetime of CH4, suggesting uncertainties in its sources and sinks. Reactive halogens substantially perturb the budget of tropospheric OH, the main CH4 loss. However, such an effect of atmospheric halogens is not considered in existing climate projections of CH4 burden and radiative forcing. Here, we demonstrate that reactive halogen chemistry increases the global CH4 lifetime by 6–9% during the 21st century. This effect arises from significant halogen-mediated decrease, mainly by iodine and bromine, in OH-driven CH4 loss that surpasses the direct Cl-induced CH4 sink. This increase in CH4 lifetime helps to reduce the gap between models and observations and results in a greater burden and radiative forcing during this century. The increase in CH4 burden due to halogens (up to 700 Tg or 8% by 2100) is equivalent to the observed atmospheric CH4 growth during the last three to four decades. Notably, the halogen-driven enhancement in CH4 radiative forcing is 0.05 W/m2 at present and is projected to increase in the future (0.06 W/m2 by 2100); such enhancement equals ~10% of present-day CH4 radiative forcing and one-third of N2O radiative forcing, the third-largest well-mixed greenhouse gas. Both direct (Cl-driven) and indirect (via OH) impacts of halogens should be included in future CH4 projections.
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