Particle Size Distributions of Oxidative Potential of Lung-Deposited Particles: Assessing Contributions from Quinones and Water-Soluble Metals

Abstract

Redox-active species in ambient particulate matter (PM) cause adverse health effects through the production of reactive oxygen species (ROS) in the human respiratory tract. However, respiratory deposition of these species and their relative contributions to oxidative potential (OP) have not been described. Size-segregated aerosols were collected during haze and nonhaze periods using a micro-orifice uniform deposit impactor sampler at an urban site in Shanghai to address this issue. Samples were analyzed for redox-active species content and PM OP. The average dithiothreitol (DTT) activity of haze samples was approximately 2.4-fold higher than that of nonhaze samples and significantly correlated with quinone and water-soluble metal concentrations. The size-specific distribution data revealed that both water-soluble OPvDTT (volume-normalized OP quantified by DTT assay) and OPmDTT (mass-normalized OP) were unimodal, peaking at 0.56-1 and 0.1-0.32 μm, respectively, due to contributions from accumulation-mode quinones and water-soluble metals. We further estimated that transition metals (mainly copper and manganese) contributed 55 ± 13% of the DTT activity while quinones accounted for only 8 ± 3%. Multiple-path particle dosimetry calculations estimated that OP deposition in the pulmonary region was mainly from accumulation-mode transition metals despite quinones having the highest DTT activity. This behavior is primarily attributed to the efficiency of deposition of transition metals in the pulmonary region being approximately 1.2-fold greater than that of quinones. These results reveal that accumulation-mode transition metals are significant contributors to the OP of deposited water-soluble particles in the pulmonary region of the lung.