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Potential of Nanoparticles and Nitrates Released to Water from Photocatalytic Pavements

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Potential of Nanoparticles and Nitrates Released to Water from Photocatalytic Pavements Construction Research Congress 2014 ©ASCE 2014 1537 Potential of Nanoparticles and Nitrates Released to Water from Photocatalytic Pavements Heather DYLLA1 and Marwa M HASSAN2 1 Louisiana State University, Department of Construction Management and Industrial Engineering 128 PFT hall, Baton Rouge, LA, 70803; Email: [email protected] 2 Louisiana State University, Department of Construction Management and Industrial Engineering 3128 PFT hall, Baton Rouge, LA, 70803; Email: [email protected] ABSTRACT Heterogeneous photocatalysis for self-cleaning and air purifying construction materials, using titanium dioxide (TiO2) nanoparticles, is a promising and fast growing technology. Much of the focus of recent research has been concentrated on understanding the photodegradation benefits such as the reduction of nitrogen oxides. Few researchers have investigated the potential adverse effects due to application of photodegradation. Potential trade-offs include the adverse environmental impact from photodegradation intermediates, photodegradation end products, or TiO2 nanoparticles released to the environment either into the atmosphere or the water. As a result, potentially harmful compounds - TiO2 nanoparticles and nitrates - released to water from photocatalytic concrete pavements were measured. The amount of nitrates eluted to water was measured after 4.5 hours of photocatalytic oxidation (PCO) of nitrogen oxide (NOx) using environmental settings, which would provide the most NOx reduced and nitrates created. After 4.5 hours of photocatalytic activity, 8.984 μmols of nitrates were released to water accounting for 49% of the theoretical amount of nitrates created. In addition, the amount of the titanium element was measured using inductive coupled plasma atomic emission spectrometry (ICP-AES). Titanium nanoparticles were not detected in any of the water samples. Keywords: nanomaterials, nanoparticle environmental exposure, nitrates, photocatalytic pavement INTRODUCTION Self-cleaning and air purifying materials, using heterogeneous photocatalysis, is fast growing evident from the increasing number of products and studies evaluating this emerging technology. Since the mid 1990’s, photocatalysts applications in construction materials have grown leading to a diverse range of nanocomposites varying from bathroom tiles, roofing materials, paints, facades, and pavements for self-cleaning and air purifying (Fujishima and Zhang 2006). Heterogeneous photocatalysis uses a semiconductor (most commonly titanium dioxide [TiO2] nanoparticles) to accelerate oxidation and reduction reactions decomposing organic and inorganic pollutants in the presence of sunlight. Furthermore, when irradiated, the surface of TiO2 become more hydrophilic enhancing the self-cleaning effect as the end products from the photocatalytic degradation can be easily adsorbed into water and washed off by rainwater (Diamanti et al. 2008). As true of most technologies, pros and cons exist. Much of the focus of recent research has been concentrated on understanding the photodegradation benefits. Few Construction Research Congress 2014 ©ASCE 2014 1538 researchers have investigated the potential adverse effects due to application of photocatalysis. In fact, researchers in a workshop on passive photocatalytic oxidation (PCO) strategies in building materials, identified this as a key research need before deployment of the technology (Berdahl and Akbari 2008). Potential trade-offs include the adverse environmental impacts from photodegradation intermediates, photodegradation end products, or TiO2 nanoparticles released to the environment either into the atmosphere or the water (Berdahl and Akbari 2008). As a result, the adverse environmental consequences of photocatalytic pavements are the subject of this paper. Potentially harmful compounds - TiO2 nanoparticles and nitrates - released to water were evaluated for photocatalytic concrete pavements used to oxidize NOx from mobile pollution sources. BACKGROUND Nitrogen oxides, 35% emitted from mobile sources, are one of the most common pollutants researched for removal potentials due to their association with acid rain, photochemical smog, and negative health impacts (Kuhns et al. 2004). Titanium dioxide has the ability to remove NOx, following the oxidation reaction scheme presented in Equations (1) and (2) with the final product as nitrates (Yu 2003): (1) (2) While nitrates are naturally found in the environment and are essential plant nutrients; in excess amounts, they can cause serious water quality problems such as eutrophication. Few studies have mentioned the amount of nitrates being released to water, stating only that the amount released is 10 times inferior to the original - pollutant level (Picada 2001). For concrete substrates, researchers believe that NO3 is absorbed by concrete substrates, due to the alkalinity of concrete (Sleiman et al. 2009, Yu 2003). Furthermore, it is theorized, but not confirmed, that the nitrates absorbed by the concrete can react with the calcium hydrate Ca(OH)2 in the concrete cement, neutralizing to Ca(NO3)2 and H2O (Li and Qian 2009). In addition to nitrates, TiO2 nanoparticles deployed from the photocatalytic layer may also be released. According to a model completed in Switzerland, the majority of the TiO2 nanoparticles are likely to be released to water or soil rather than to the air (Mueller et al., 2008). Yet, nanoscale TiO2 is one of the most manufactured and greatest used of all nanoparticles, few studies have shown the release of nano- TiO2 into the natural environment (Kaegi et al., 2009). This absence of exposure data for current nanomaterial containing products has been widely reported as a significant research gap by nanoparticle toxicologists (Stern and McNeil 2008). Uses of TiO2 for photocatalyst cements for both building facades and pavements have the potential of releasing TiO2 due to abrasion. For example, TiO2 used as a whitening agent in paints exhibits chalking effects exposing TiO2 particles to the surface (Kaegi et al., 2009). Furthermore, abrasion due to repeated traffic on photocatalytic pavements potentially releases TiO2 nanoparticles as well (Hassan et al., 2010). One study by Kaegi et al., illustrated the release of synthetic TiO2 nanoparticles, 3.5 x 108 particles/L, from exterior applications to the aquatic Construction Research Congress 2014 ©ASCE 2014 1539 environments. This study was the first time that showed significant amounts of manufactured TiO2 released into the aquatic systems. TiO2 was released first as agglomerates in direct façade storm water runoff and was degraded as it reached the inlet of the urban runoff storm water systems suggesting that the organic matrix was either dissolved or degraded during transport (Kaegi et al., 2009). The toxicity of TiO2 nanoparticles is not completely understood. The toxicity of nanoparticles is dependent on several characteristics; particle size, surface area, metals/impurities, surface charge, morphology, crystallinity, and solubility in biological fluids, some of which, are even difficult to measure (Isaacs 2009). Furthermore, nanoparticles are ubiquitous formed naturally, incidentally or artificially. For example, natural TiO2, nanoparticles were found in river water (Wigginton et al., 2007). Over the years, ecosystems have adapted to “cohabitate” with these nanoparticles; however, many details are still unknown such as the relative exposure levels especially since the difference between these three types of nanoparticles are blurred (Wiesner et al., 2009). As a result, it is questionable whether one will be able to distinguish one type from the other two making it difficult to access the risks of manufactured nanoparticles (Wiesner et al., 2009). Consequently, there is little understanding of the possible consequences when using manufactured photocatalytic nanoparticles. To avoid major negative implications, significant effort needs to be brought forward to quantify both the toxicity and exposure potential for these nanoparticles (Robichaud et al. 2009, Lee et al. 2009). METHODOLOGY This study was divided into two parts; (1) to quantify how much nitrates are eluted into water and (2) to quantify and characterize TiO2 nanoparticles eluted into water. Part one of the study was to investigate the worse case scenario of how much nitrates are eluted into water from photocatalytic pavements. Water samples were analyzed from photocatalytic pavements and compared to water samples from concrete pavement controls before and after PCO of NOx. The nitrates were quantified using the automated cadmium reduction test in accordance to EPA Method 353.2 (EPA 1993). The difference in nitrates eluted from photocatalytic pavements and the concrete control is due to the PCO of NOx. Part 2 of the study investigated whether engineered TiO2 nanoparticles used in photocatalytic pavements were released into water. To this end, water samples from two different types of photocatalytic concrete pavements (photocatalytic mortar overlays and photocatalytic spray coats), were analyzed and compared to water samples from typical concrete pavement (control). These water samples were quantitatively analyzed using inductive coupled plasma atomic emission spectrometry (ICP-AES) in accordance to EPA Method 6010c (EPA 2007). Concrete Pavement Samples Two different types of photocatalytic concrete pavements were investigated; photocatalytic mortar overlays, and photocatalytic spray coats (Part 2 only). The photocatalytic coating was applied to a concrete base with
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