Department of Chemistry, Syracuse University, Syracuse, New York, USA.
Department of Civil and Environmental Engineering, Rice University, Houston, Texas, USA.
Indoor Air. 2022 Jan;32(1):e12964. doi: 10.1111/ina.12966. Epub 2021 Dec 2.
We made intensive measurements of wavelength-resolved spectral irradiance in a test house during the HOMEChem campaign and report diurnal profiles and two-dimensional spatial distribution of photolysis rate constants (J) of several important indoor photolabile gases. Results show that sunlight entering through windows, which was the dominant source of ultraviolet (UV) light in this house, led to clear diurnal cycles, and large time- and location-dependent variations in local gas-phase photochemical activity. Local J values of several key indoor gases under direct solar illumination were 1.8-7.4 times larger-and more strongly dependent on time, solar zenith angle, and incident angle of sunlight relative to the window-than under diffuse sunlight. Photolysis rate constants were highly spatially heterogeneous and fast photochemical reactions in the gas phase were generally confined to within tens of cm of the region that were directly sunlit. Opening windows increased UV photon fluxes by 3 times and increased predicted local hydroxyl radical (OH) concentrations in the sunlit region by 4.5 times to 3.2 × 10 molec cm due to higher J values and increased contribution from O photolysis. These results can be used to improve the treatment of photochemistry in indoor chemistry models and are a valuable resource for future studies that use the publicly available HOMEChem measurements.
我们在 HOMEChem 活动期间对测试房屋内的波长分辨光谱辐照度进行了密集测量,并报告了几种重要室内光解气体的光解率常数 (J) 的日变化曲线和二维空间分布。结果表明,通过窗户进入的阳光是该房屋中紫外线 (UV) 光的主要来源,导致明显的日变化,以及局部气相光化学活性随时间和位置的强烈变化。在直接阳光照射下,几种关键室内气体的局部 J 值比漫射阳光下大 1.8-7.4 倍,并且更强烈地依赖于时间、太阳天顶角和阳光相对于窗户的入射角。光解率常数在空间上高度不均匀,气相中的快速光化学反应通常局限于直接阳光照射区域内的几十厘米范围内。由于 J 值更高且 O 光解的贡献增加,打开窗户使 UV 光子通量增加了 3 倍,并使受阳光照射区域的预测局部羟基自由基 (OH) 浓度增加了 4.5 倍,达到 3.2×10 摩尔·cm 。这些结果可用于改进室内化学模型中光化学的处理方式,并且是未来使用公开可用的 HOMEChem 测量值进行研究的宝贵资源。