Black soiling of an architectural limestone during two-year term exposure to urban air in the city of Granada (S Spain)

A two-year term aging test was carried out on a building limestone under different urban conditions in the city of Granada (Southern Spain) to assess its Cultural Heritage sustainability. For this purpose stone tablets were placed vertically at four sites with contrasting local pollution micro-environments and exposure conditions (rain-sheltered and unsheltered). The back (rain-sheltered) and the front (rain-unsheltered) faces of the stone tablets were studied for each site. The soiling process (surface blackening) was monitored through lightness (ΔL*) and chroma changes (ΔC*). Additionally atmospheric particles deposited on the stone surfaces and on PM10 filters during the exposure time were studied through a multianalytical approach including scanning electron microscopy (SEM-EDX), transmission electron microscopy (TEM) and micro-Raman spectroscopy. The identified atmospheric particles (responsible for stone soiling) were mainly soot and soil dust particles; also fly ash and aged salt particles were found. The soiling process was related to surface texture, exposure conditions and proximity to dense traffic streets. On the front faces of all stones, black soiling and surface roughness promoted by differential erosion between micritic and sparitic calcite were noticed. Moreover, it was found that surface roughness enhanced a feedback process that triggers further black soiling. The calculated effective area coverage (EAC) by light absorbing dust ranged from 10.2 to 20.4%, exceeding by far the established value of 2% EAC (limit perceptible to the human eye). Soiling coefficients (SC) were estimated based on square-root and bounded exponential fittings. Estimated black carbon (BC) concentration resulted in relatively similar SC for all studied sites and thus predicts the soiling process better than using particulate matter (PM10) concentration. ► A two-year term aging test was carried out on a building limestone under different urban conditions. ► The soiling process depends on surface texture and local micro-environments. ► Stone soiling was due to soot and soil, dust particles and fly ash. ► The estimated soiling coefficients were slightly lower than in other cities of Spain. ► Gypsum crust was developed during the first year of exposure.