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Harmful algal blooms (HABs) in lakes and estuaries, caused by cyanobacteria, pose various threats to humans and the environment. Cyanobacteria produce microcystins (MCs) that make animals and people sick. Once airborne, cyanobacterial aerosols are rapidly transformed through heterogeneous reactions with atmospheric oxidants, which tend to occur much faster in air than in water. The important aspects of these transformations include the degradation of MCs and the production of reactive oxygen species (ROS) from oxidized organic matter (OM) in cyanobacterial aerosol. In this study, MCs in aerosols and water samples, collected in lakes (Lake Okeechobee, Georges Lake, and Doctors Lake) of Florida during HABs, were measured using enzyme-linked immunosorbent assay kits. Organic hydroperoxides (OHP) and the oxidative potential (OP) associated with aerosols collected at Doctors Lake were measured with 4-nitrophenylboronic acid and dithiothreitol assays, respectively. The decay of MCs and the evolution of ROS in cyanobacterial aerosols were also demonstrated in an outdoor chamber under ambient sunlight. MC concentrations (0.4–2.1 μg/L) during HAB periods were higher than the US EPA guideline (0.3 μg/L for pre-school age and 1.6 μg/L for school-age and above). Airborne MC concentrations ranged from 0.2 to 5.7 ng/m3. Regulations for airborne MC concentrations are yet to be established. In both field and chamber data, MCs decomposed but ROS substantially increased as aerosols atmospherically oxidized. Aerosolized OM concentrations during HABs were higher than those in dormant periods. OM in cyanobacterial aerosols was enriched at estuary Doctors Lake with high inorganic salt concentrations due to salting-out of water-soluble organics into lake-surface layers. Aerosolized OM concentrations were positively corelated to OP and OHP (r = 0.96 and 0.85, respectively) at Doctors Lake suggesting that cyanobacterial aerosols might adversely influence respiratory health. The longitudinal health impacts of aerosolized cyanobacteria emitted from HABs should be investigated in the future. 

Abstract Red tide is caused by the accumulation of Karenia (K.) brevis, which produces brevetoxin (BTx), a neurotoxin. Excreted BTx is incorporated into sea spray aerosol (SSA), which is created from the bursting of bubbles at the ocean’s surface. For the first time, this study measures the enrichment factor of BTx in K. brevis algal aerosol. During red-tide events in 2021 and 2022, aerosol and water samples were collected from Gulf Coast beaches in Southwest Florida with various levels of K. brevis growth. The concentrations of BTx in SSA were measured using an enzyme-linked immunosorbent assay kit. The concentrations of both aerosolized BTx and organic matter (OM) were normalized using that of sodium ions and were shown to be significantly higher than those observed in seawater. Lipophilic BTx is present in SSA at concentrations that are 2-4 orders of magnitude higher than seawater, and 1-2 orders of magnitude higher than concentrations of OM in SSA. Enrichment of aerosolized BTx was also simulated in the algal culture tank with two different aerosol generation methods. The estimated activity coefficient (order of 1019) of BTx in bulk seawater using the inorganic thermodynamic model indicates very poor solubility of BTx in seawater and supports its enrichment in ocean surfaces and SSA. Examining the enrichment factors of BTx and organic matter in SSA contributes to our comprehension of the potential respiratory challenges posed by inhaled algal aerosols during red tide occurrences. In addition, enriched BTx in the uppermost layer of the ocean during red tide blooms can adversely influence animals that inhabit in tide flats with neurological and respiratory impacts.