Integrated impacts of turbulent mixing and NOX-O3 photochemistry on reactive pollutant dispersion and intake fraction in shallow and deep street canyons.

We employ computational fluid dynamics (CFD) simulations with NO-NO2-O3 chemistry to investigate the impacts of aspect ratios (H/W = 1,3,5), elevated-building design, wind catchers and two background ozone concentrations ([O3]b = 100/20 ppb) on reactive pollutant dispersion in two-dimensional (2D) street canyons. Personal intake fraction of NO2 (P_IFNO2) and its spatial mean value in entire street (i.e. street intake fraction <P_IFNO2>) are calculated to quantify pollutant exposure in near-road buildings. Chemical reaction contribution of NO2 exposure (CRC<P_IF>), O3 depletion rate (dozone) and photostationary state defect (δps) are used to analyze the interplay of turbulent and chemical processes. As H/W increases from 1, 3 to 5 with [O3]b = 100 ppb, the flow pattern turns from single-main-vortex structure to two-counter-rotating-vortex structure, and pedestrian-level velocity becomes 1-2 orders smaller. The high-dozone regions and low-|δps| regions get larger with more complete chemical reactions. Consequently, passive <P_IFNO2> rises 1 order (4.09-5.71 ppm to 41.76 ppm), but reactive <P_IFNO2> only increases several times (17.80-21.28 ppm to 58.50 ppm) and the contribution of chemistry (CRC<P_IF>) decreases with higher H/W. Thus, chemistry raises <P_IFNO2 > more effectively in shallow street canyons (H/W = 1-3). In deep street canyons (H/W = 5), elevated-building design and wind catchers destroy two-counter-rotating-vortex structure, improve street ventilation and reduce passive <P_IFNO2> by 2 and 1 orders (41.76 ppm to 0.38-5.16 ppm), however they only reduce reactive <P_IFNO2> by about 97.5% and 75% (58.50 ppm to 1.61-14.48 ppm). Such building techniques induce lower O3 depletion rate but greater chemical contribution. Finally, raising [O3]b from 20 to 100 ppb causes greater O3 depletion rate and chemical contribution and produces larger <P_IFNO2>. For deep street canyons, the impact of higher [O3]b on <P_IFNO2> is weaker than that in shallow street canyons, while it becomes stronger when fixing elevated-building design and wind catchers. This study provides some innovative findings on reactive pollutant exposure in 2D street canyons and offers effective CFD methodologies to evaluate pollutant exposure with more complicated chemistry and urban configurations.