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Bed Flow Photoreactor Experiments to Assess the Photocatalytic Nitrogen Oxides Abatement Under Simulated Atmospheric Conditions F

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Bed Flow Photoreactor Experiments to Assess the Photocatalytic Nitrogen Oxides Abatement Under Simulated Atmospheric Conditions F Bed flow photoreactor experiments to assess the photocatalytic nitrogen oxides abatement under simulated atmospheric conditions F. Mothes, S. Ifang, M. Gallus, B. Golly, A. Boreave, R. Kurtenbach, J. Kleffmann, C. George, H. Herrmann To cite this version: F. Mothes, S. Ifang, M. Gallus, B. Golly, A. Boreave, et al.. Bed flow photoreactor experiments to assess the photocatalytic nitrogen oxides abatement under simulated atmospheric conditions. Applied Catalysis B: Environmental, Elsevier, 2018, 231 (—), pp.161-172. 10.1016/j.apcatb.2018.03.010. hal-01868871 HAL Id: hal-01868871 https://hal.archives-ouvertes.fr/hal-01868871 Submitted on 18 Nov 2020 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Distributed under a Creative Commons Attribution - NonCommercial| 4.0 International License Applied Catalysis B: Environmental 231 (2018) 161–172 Contents lists available at ScienceDirect Applied Catalysis B: Environmental journal homepage: www.elsevier.com/locate/apcatb Bed flow photoreactor experiments to assess the photocatalytic nitrogen T oxides abatement under simulated atmospheric conditions F. Mothesa, S. Ifangb, M. Gallusb, B. Gollyc, A. Boréavec, R. Kurtenbachb, J. Kleffmannb, ⁎ C. Georgec, H. Herrmanna, a Leibniz-Institute for Tropospheric Research (TROPOS), Atmospheric Chemistry Department (ACD), Permoserstraße 15, 04318 Leipzig, Germany b Institute for Atmospheric & Environmental Research, Bergische Universität Wuppertal (BUW), Gaußstr. 20, 42119 Wuppertal, Germany c Univ Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, F-69626, Villeurbanne, France ARTICLE INFO ABSTRACT Keywords: Small scale bed flow photoreactor experiments were performed to assess the photocatalytic performance of Heterogeneous photocatalysis cement-based TiO2-containing materials for NOx reduction through the determination of kinetic parameters Titanium dioxide under variation of the experimental conditions (relative humidity, flow rate, mixing ratio and light intensity) and Cement-based material monitoring of potential reaction products in the gas phase and the aqueous extract of the surface. NO x The results clearly demonstrated the general potential of the tested material to photocatalytically remediate Bed flow reactor gas phase NOx by conversion into nitrite and nitrate as identified reaction products at the surface. The measured −5 uptake coefficients for NO and NO2 under atmospheric relevant conditions were in the range of 5 × 10 with a − corresponding surface deposition velocity of about 0.5 cm s 1. However, it became also clear that the photo- catalytic activity is in part significantly dependent on the experimental conditions. The relative humidity and the mixing ratio of the air pollutant were identified as the most important parameters. In addition, under certain conditions, a renoxification process can occur. The comprehensive results of the present study are discussed in detail to develop recommendations for a possible future application of this technique to improve urban air quality. 1. Introduction combination with volatile organic compounds (VOCs), to the formation of these most problematic secondary air pollutants. Sources for NOx are Clean air is essential to human health and for the intactness of the high temperature combustion processes, mainly emitted by power environment. Since the industrial revolution, however, the quality of plants (21% by energy industry) and combustion engines (47% by the the air that people breathe has deteriorated considerably as a result of transport sector) [2]. To protect human health, the EU Air Quality Di- human activities. The need to deliver cleaner air has been recognized rective (EU, 2008c, Directive 2008/50/EC) introduced a threshold −3 for several decades with action having been taken at national, EU-level value for NO2 (annual mean 40 μgm ) which is often exceeded by the and world-wide levels, not at least through multilateral international accumulated car emissions at traffic hotspots in urban areas. In 2014, conventions and activities. Despite significant reduction of pollutant 94% of the measuring stations with values above the limit were traffic emissions, serious air pollution problems still persist [1]. Against this related [1]. backdrop, the EU adopted in 2013 the “New Clean Air Package”, in- Among new technical “solutions” designed for large dissemination cluding the update of legal monitoring of pollutant emissions by in- over the public space, new photocatalytic building and coating mate- dustry, transport, power plants and agricultural activities [2]. The long- rials have been proposed as a “green” remediation technology for NOx term objective is to achieve levels of air pollution that do not lead to and VOCs in the polluted urban environment [3,4]. These commercial unacceptable harm to human health and the environment until 2050. products are based on the photocatalytic properties of a thin layer of the EU-action has therefore focused on establishing minimum air quality semiconductor titanium dioxide (TiO2) deposited at the surface of the standards for ambient air to tackle the problems of particulate matter material (such as glass, pavement, etc.) or embedded in the substrate (PM) and ground level ozone (O3). In this context, nitrogen oxides (i.e., e.g., in paints or concrete and their depollution performance has al- NOx =NO+NO2) play an important role, since they contribute, in ready been assessed in numerous studies [5–21]. ⁎ Corresponding author. E-mail address: [email protected] (H. Herrmann). https://doi.org/10.1016/j.apcatb.2018.03.010 Received 6 February 2018; Accepted 3 March 2018 Available online 04 March 2018 0926-3373/ © 2018 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/BY/4.0/). F. Mothes et al. Applied Catalysis B: Environmental 231 (2018) 161–172 Fig. 1. Schematic overview of the experimental set-up, MFC = mass flow controller. The interaction of the TiO2 based photocatalyst and light of ap- 2. Experimental propriate wavelength (UV-light, ≤400 nm, [22]) results in a charge separation according to Hoffmann, et al. [23]: 2.1. Sample preparation TiO+→ hν h+− + e fs range (R-1) 2 vb cb Two different photocatalytically active cement-based coating ma- Here, an electron from the valence band of the semiconductor is pro- terials prepared by the manufacturer CTG Italcementi Group (based on − ® moted into the conduction band (ecb ), leaving a hole in the valence the TX Active technology, [45]) have been investigated and compared + band (hvb ). Both at the surface, or, through their diffusion through the with an inactive reference material (Ri), which had the same compo- particle bulk, both photogenerated charge carriers might recombine sition as the active materials but without the photocatalyst TiO2. The (null cycle) while only at the surface they can react with adsorbed re- photocatalytically active materials contained different amounts of TiO2 actants creating radicals. For example, the reaction with oxygen and (approximate composition: A = 0.3% and B = 1.0% wt.) and approxi- − water lead to the formation of highly reactive radicals such as O2 /HO2 mately 1.0 ± 0.3% of organic carbon (measuring protocol given in SI and OH proven by measurements using, e.g., electron paramagnetic 1) as organic additive/binding material. To investigate the cement- resonance (EPR) [24], cavity ring down spectroscopy (CRDS) [25]or based coating material it was mixed with ultra-pure water (Milli‐Q laser-induced fluorescence (LIF) [26–29]. These reactive oxygen species gradient A 10, 18.2 MΩ cm, 3 ppb TOC, Millipore) using a water to solid (ROS) enable irradiated TiO2, especially in its most active form Anatase ratio of w/s = 0.175 and subsequently applied on sand blasted glass [30], to degrade adsorbed NOx and VOCs [31,32]. plates (dimensions: 5 × 40 cm) with a final surface thickness of about Based on laboratory studies, it is generally concluded that NOx is 3-4 mm. After a curing period of approximately one month, the coated quantitatively converted into nitrate anions [6,11,33–35], which re- glass plates were cleaned with ultra-pure water and dried under clean main adsorbed on the surface until washed off, for example by rain, air conditions to avoid a surface contamination due to adsorption of whereas the VOCs are mostly mineralized to carbon dioxide and water chemical compounds or dirt/dust particles from ambient air. [36,37]. However, some recent studies on pure photocatalysts and on self-cleaning window glass also observed the formation of harmful in- termediates, for example nitrous acid (HONO) [6,38,39], which is even 2.2. Experimental set-up and procedure more harmful than the primary reactants NO and NO2. In addition, renoxification originating from adsorbed nitrate, proposed by the For the qualitative and quantitative assessment of the photocatalytic photocatalytic formation of the nitrate radical (NO3) on TiO2, was re- efficiency of such materials, different standard methods (UNI, ISO) re- cently observed in laboratory
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