References of "Mahy, Julien"
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See detailHighly efficient doped nanocristalline TiO2 for water Treatment
Mahy, Julien ULg; Léonard, Géraldine ULg; Zubiaur, Anthony ULg et al

Conference (2017, July 13)

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See detailAqueous sol-gel synthesis and film deposition methods for the large-scale manufacture of coated steel with self-cleaning properties
Mahy, Julien ULg; Léonard, Géraldine ULg; Pirard, Sophie ULg et al

in Journal of Sol-Gel Science and Technology (2017), 81(1), 27-35

A process has been developed to enable the large scale production of pure TiO2 films deposited on 316L stainless steel in order to get an easy-to-clean surface. This large scale process requires an easy ... [more ▼]

A process has been developed to enable the large scale production of pure TiO2 films deposited on 316L stainless steel in order to get an easy-to-clean surface. This large scale process requires an easy aqueous sol-gel procedure for the synthesis of the TiO2 sol. This synthesis has been simplified to facilitate the extrapolation towards an industrial scale. Results of TEM, photocatalytic properties, film hydrophilicity, and texture obtained with the simplified aqueous sol-gel synthesis (IsoP-TiO2 synthesis) show similar properties to those obtained with the standard aqueous sol-gel synthesis of TiO2 (HAc-TiO2 synthesis) developed previously. Only X-Ray Diffraction patterns showed differences, with the presence of anatase-brookite phases in IsoP-TiO2 synthesis while anatase phase only was observed in HAc-TiO2 synthesis. Both the aqueous sol-gel synthesis of pure TiO2 and the film deposition on steel by roll-coating have been successfully extrapolated to a larger scale. The photocatalytic activity and the hydrophilicity of the film were found to be unchanged when compared to films produced at a laboratory scale, thus validating the production of an efficient easy-to-clean material. Although some problems are still to be solved, this study is a hopeful first step in the development of a large scale process for self-cleaning steel production. [less ▲]

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See detailEthylene polymerization and hydrodechlorination of 1,2-dichloroethane mediated by nickel(II) covalently anchored to silica xerogels
Mahy, Julien ULg; Claude, Vincent ULg; Sacco, Luigi et al

in Journal of Sol-Gel Science and Technology (2017), 81(1), 59-68

Ni/SiO2 cogelled xerogel catalysts have been prepared in ethanol containing nickel acetylacetonate, tetraethoxysilane (TEOS), an aqueous ammonia solution of 0.54 mol L-1 and either a commercial sylilated ... [more ▼]

Ni/SiO2 cogelled xerogel catalysts have been prepared in ethanol containing nickel acetylacetonate, tetraethoxysilane (TEOS), an aqueous ammonia solution of 0.54 mol L-1 and either a commercial sylilated ligand, 3-(2-aminoethyl)aminopropyltrimethoxysilane (EDAPMS), or a home-made new silylated pyrazolypyridine ligands, respectively 2-[4-[3-(trimethoxysilyl)propyl]-3,5-dimethyl-1H-pyrazol-1-yl]pyridine (MS-PzPy) and 2-[4-[3-(trimethoxysilyl)propyl]-3,5-dimethyl-1H-pyrazol-1-yl]-6-methylpyridine (MS-PzPyMe), able to form a chelate with a metal ion such as Ni2+. All samples form homogeneous and very highly dispersed Ni/SiO2 cogelled xerogel catalysts. The resulting catalysts are composed of nickel nanoparticles with a diameter of about 2.8 nm, located inside primary silica particles exhibiting a monodisperse microporous distribution. The silylated organic ligand has a strong influence on the textural properties of cogelled xerogel catalysts, both before and after calcination and reduction steps. Changing the nature of the silylated ligand permits tailoring textural properties such as pore volume, pore size and surface area. Homogenous nickel complexes synthesized from pyrazolylpyridine derivatives are inactive for ethylene polymerization. In opposite, heterogenous nickel-based catalysts onto silica xerogel synthesized from pyrazolylpyridine derivatives bearing a tethered trialkoxysilyl group allow increasing ethylene polymerization activity. Although nickel nanoparticles are located inside the silica crystallites, their complete accessibility, via the micropore network, has been shown. For 1,2-dichloroethane hydrodechlorination over Ni/SiO2 catalysts, the conversion of 1,2-dichloroethane is high at the temperature of 350°C and mainly ethane is produced. [less ▲]

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See detailStudy of the photocatalytic activity of Fe3+, Cr3+, La3+ and Eu3+ single-doped and co-doped TiO2 catalysts produced by aqueous sol-gel processing
Malengreaux, Charline; Pirard, Sophie ULg; Léonard, Géraldine ULg et al

in Journal of Alloys and Compounds (2017), 691

An aqueous sol-gel process, previously developed for producing undoped and Cu2+, Ni2+, Zn2+ or Pb2+ doped TiO2 photocatalysts with remarkably high photocatalytic activity without requiring any calcination ... [more ▼]

An aqueous sol-gel process, previously developed for producing undoped and Cu2+, Ni2+, Zn2+ or Pb2+ doped TiO2 photocatalysts with remarkably high photocatalytic activity without requiring any calcination step, has been adapted to produce Fe3+, Cr3+, La3+ or Eu3+ single-doped TiO2 photocatalysts as well as La3+-Fe3+ and Eu3+-Fe3+ co-doped TiO2 catalysts. The physicochemical properties of the obtained catalysts have been characterized using a suite of complementary techniques, including ICP-AES, XRD, UV-Vis spectroscopy, nitrogen adsorption-desorption and Fe-57 Mössbauer. The active crystalline phase is obtained without requiring any calcination step and all the different catalysts are composed of nanocrystallites of anatase with a size of 6-7 nm and a high specific surface area varying from 181 to 298 m² g-1. In this study, the effect of the NO3:Ti(IV) mole ratio used to induce the peptisation reaction during the synthesis has been studied and the results revealed that this ratio can influence significantly the textural properties of the resulting catalyst. A screening of the photocatalytic activity of the undoped and Fe3+, Cr3+, La3+ or Eu3+ single-doped and co-doped photocatalysts has been performed by evaluating the degradation of 4-nitrophenol under UV-Visible light (330 nm < λ < 800 nm). This study suggests that the photocatalytic activity is significantly influenced by the dopant nature and content with an optimal dopant content being observed in the case of Fe3+ or La3+ single-doped as well as in the case of La3+-Fe3+ and Eu3+-Fe3+ co-doped catalysts. In the case of Cr3+ single-doped catalysts, a detrimental effect of the dopant on the photocatalytic degradation of 4-nitrophenol has been observed while no significant influence of the dopant has been detected in the case of Eu3+ single-doped catalysts. The role of the different dopants in modulating the photocatalytic activity is discussed. [less ▲]

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See detailTowards a large scale aqueous sol-gel synthesis of doped TiO2: Study of various metallic dopings for the photocatalytic degradation of p-nitrophenol
Mahy, Julien ULg; Lambert, Stéphanie ULg; Léonard, Géraldine ULg et al

in Journal of Photochemistry and Photobiology A : Chemistry (2016), 329

In this paper, an easy aqueous sol-gel synthesis developed previously by Mahy et al. [J. Sol-Gel Sci. Technol. (2016)] is adapted to produce highly active TiO2 catalysts doped with Fe3+, Ag+, Cu2+, Zn2 ... [more ▼]

In this paper, an easy aqueous sol-gel synthesis developed previously by Mahy et al. [J. Sol-Gel Sci. Technol. (2016)] is adapted to produce highly active TiO2 catalysts doped with Fe3+, Ag+, Cu2+, Zn2+, Cr3+, Al3+, Mn2+, and Co2+ ions and Pt metallic nanoparticles. Samples are characterized by inductively coupled plasma–atomic emission spectroscopy (ICP-AES), X-ray diffraction (XRD), Mössbauer spectroscopy, transmission electron microscopy (TEM), nitrogen adsorption–desorption measurements and diffuse reflectance spectroscopy measurements. Results show that the samples are composed of anatase-brookite TiO2 nanoparticles with a spherical shape and mean diameter of around 5-8 nm and a surface area of between about 150 - 250 m2 g-1. In each doped sample, the dopant is present in the form added during the synthesis, given that the sample has not undergone any particular treatment. Photoactivity tests show improvement in catalyst activity for Fe3+, Ag+, Cu2+, Zn2+, and Al3+ ion and Pt metallic nanoparticle dopants, while a decrease of activity is obtained for Cr3+, Mn2+ and Co2+ ion dopants. For some dopants, the activity of TiO2 doped with metallic ions and synthesized from the aqueous sol-gel process is equal or superior to the activity of the commercial photocatalyst Degussa P25. Some mechanisms are proposed to explain these modifications of activity with doping. Furthermore, cost comparison at laboratory scale showed that Zn and Cu nitrate salt dopings are clearly less expensive for a halogen light (UV/visible) or low energy light enhanced catalyst and may be considered for industrial applications. Using this method, a large scale Zn-doped TiO2 photocatalyst is synthesized with properties homologous to the lab-scale product. Results show that the aqueous sol-gel synthesis developed previously can be easily adapted for doping in order to produce an up-scalable synthesis. [less ▲]

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See detailAg/SiO2 and Cu/SiO2 cogelled xerogel catalysts for benzene combustion and 2-butanol deshydrogenation
Mahy, Julien ULg; Claude, Vincent ULg; Tasseroul, Ludivine ULg et al

Poster (2016, June 08)

Tars are recognized as major impurities when biomass is gazified into Syngas (mixture CO + H2) or when the methane reforming was produced from sustainaible reagents [1]. Therefore, fundamental knowledge ... [more ▼]

Tars are recognized as major impurities when biomass is gazified into Syngas (mixture CO + H2) or when the methane reforming was produced from sustainaible reagents [1]. Therefore, fundamental knowledge of catalytic oxidation and deshydrogenation mechanisms can be valuable to develop effective methods to control syngas or methane pollution. A very important concern about cogelled catalysts is the accessibility of the active centers. Because the silver and copper is located inside silica particles, there is a risk that it may not be accessible. In the case of benzene oxidation, it was observed that the specific activity (mol s-1 g-1Ag) of Ag/SiO2 and Cu/SiO2 catalysts increases when the silver or copper loading decreases (Fig. 1). In fact, visual observations by TEM showed that in samples Ag0.25, Ag0.45, Ag1.05 and Cu1.00, there are not silver or copper particles located on silica particles external surface and then the metal dispersion values are greater in these samples. So, it is the proof that Ag and Cu particles located inside the silica particles are accessible for benzene in this catalytic system. In the case of 2-butanol dehydrogenation, the specific activity of Cu/SiO2 catalysts increases when the copper loading increases or when the metal dispersion values decreases (Fig. 2). However, in Cu1.00 sample, copper particles inside silica particles only are observed by TEM. It seems that these metallic particles are accessible for 2-butanol in this catalytic system. [less ▲]

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See detailDevelopment of an easy aqueous sol-gel synthesis for large-scale film deposition methods for the manufacture of coated steel with self-cleaning properties
Mahy, Julien ULg; Léonard, Géraldine ULg; Pirard, Sophie ULg et al

Conference (2016, May 20)

In this work, a global process has been developed to produce at a large scale pure TiO2 films deposited on steel in order to get an easy-to-clean surface. This large scale process implies an easy aqueous ... [more ▼]

In this work, a global process has been developed to produce at a large scale pure TiO2 films deposited on steel in order to get an easy-to-clean surface. This large scale process implies an easy aqueous sol-gel process for the synthesis of the TiO2 sol. This synthesis [1] has been simplified to make easier the extrapolation towards an industrial scale. Results of TEM, photocatalytic properties, film hydrophilicity, and texture obtained with the simplified aqueous sol-gel synthesis (IsoP-TiO2 synthesis) show similar properties than those obtained with the standard aqueous sol-gel synthesis of TiO2 developed previously (HAc-TiO2 synthesis [2]). Only XRD patterns were slightly different with the presence of anatase-brookite phases in IsoP-TiO2 synthesis while anatase phase only was observed in HAc-TiO2 synthesis. Both the aqueous sol-gel synthesis of pure TiO2 and the film deposition on steel by roll-coating have been successfully extrapolated to a larger scale. Indeed, the deposition was done on a pilot line, the steel substrate is 25 cm width, and the band length is 800 m. The coating was deposited at line speed ranging from 30 to 120 m.min-1.The photocatalytic activity and the hydrophilicity of the film were found to be unchanged compared to the films produced at a laboratory scale, thus validating the production of an efficient easy-to-clean material. Even if some problems have still to be solved, this study is a hopeful first step in the development of a large scale process for self-cleaning steel production. [1] S. Mahshid, M. Askari, M.S. Ghamsari, J. Mater. Process. Technol. 189 (2007) 296–300 [2] C.M. Malengreaux, S. Douven, D. Poelman, B. Heinrichs, J.R. Bartlett, J. Sol-Gel Sci. Technol. 71 (2014) 557–570 [less ▲]

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See detailEfficient P- and Ag-doped titania for the photocatalytic degradation of waste water organic pollutants
Bodson, Céline ULg; Heinrichs, Benoît ULg; Tasseroul, Ludivine ULg et al

in Journal of Alloys & Compounds (2016), 682

In this work, physico-chemical properties and photocatalytic activity of three types of dried or dried and calcined TiO2 materials, synthesized by the cogelation method, were studied: (i) a pure TiO2 ... [more ▼]

In this work, physico-chemical properties and photocatalytic activity of three types of dried or dried and calcined TiO2 materials, synthesized by the cogelation method, were studied: (i) a pure TiO2 xerogel ; (ii) TiO2 xerogels doped with Ag ; (iii) TiO2 xerogels co-doped with Ag and P. The presence of silver nanoparticles was observed by transmission electron microscopy (TEM) and the oxidation state of silver after calcination was examined by temperature-programmed reduction (TPR) measurements. The physico-chemical properties of xerogels were characterized by X-ray diffraction (XRD), diffuse reflectance UV-Vis spectroscopy (DR UV-Vis) and from nitrogen adsorption-desorption isotherms. The photocatalytic activity of the samples was quantified for the p-nitrophenol degradation under visible light. [less ▲]

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See detailFe3+/Iron Oxide/SiO2 Xerogel Catalysts for p-nitrophenol Degradation by Photo-Fenton Effects: Influence of Thermal Treatment on Catalysts Texture
Mahy, Julien ULg; Tasseroul, Ludivine ULg; Herlitscke, Marcus et al

in Materials Today: Proceedings (2016), 3(2), 464-469

Three iron xerogel catalysts were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ... [more ▼]

Three iron xerogel catalysts were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ions. Four thermal treatments were applied to catalysts: drying, drying-autoclaving, calcination and calcination-autoclaving. Textural characterizations show that the specific surface area is increased by calcination while materials microporosity completely collapse when using autoclaving. Based on Mössbauer spectroscopy and magnetometry measurements, only Fe3+ species were observed in xerogel catalysts. The photo-Fenton effect of these catalysts was evaluated on the degradation of p-nitrophenol in aqueous media. In the presence of H2O2, results show that this effect reachs 99% of degradation after 24 h. Mössbauer and catalytic tests are presented in another paper. [less ▲]

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See detailDevelopment by the sol–gel process of highly dispersed Ni–Cu/SiO2 xerogel catalysts for selective 1,2-dichloroethane hydrodechlorination into ethylene
Pirard, Sophie ULg; Mahy, Julien ULg; Pirard, Jean-Paul ULg et al

in Microporous and Mesoporous Materials (2015), 209

Ni–Cu/SiO2 xerogel catalysts have been synthesized by cogelation of industrial tetraethoxysilane (Dynasil) and chelates of Ni and Cu with industrial 3-(2-aminoethylamino)propyltrimethoxysilane (Dynasylan ... [more ▼]

Ni–Cu/SiO2 xerogel catalysts have been synthesized by cogelation of industrial tetraethoxysilane (Dynasil) and chelates of Ni and Cu with industrial 3-(2-aminoethylamino)propyltrimethoxysilane (Dynasylan DAMO) in industrial ethanol denatured with diethyl phthalate. Despite the use of industrial grade reagents, highly dispersed bimetallic Ni–Cu/SiO2 xerogel catalysts were obtained. These samples are composed of completely accessible Ni–Cu alloy crystallites with sizes of 1.6–3.4 nm located inside silica particles exhibiting a monodisperse microporous distribution. It appears that the bimetallic complex acts as a nucleation agent in the formation of silica particles. The combination of results obtained from the calculation of the metal ratio in catalysts, H2 chemisorption and transmission electron microscopy allowed calculating the surface composition of the nickel–copper particles in Ni–Cu/SiO2 cogelled xerogel catalysts. Values obtained indicate a very pronounced surface enrichment with copper. While 1,2-dichloroethane hydrodechlorination over pure nickel mainly produces ethane, increasing copper content in bimetallic catalysts results in an increase in ethylene selectivity. The specific consumption rate of 1,2-dichloroethane decreases when copper loading increases. The turnover frequency, that is, the number of catalytic cycle per active site (nickel atom and its surrounding copper atoms) and per second, seems to be independent of surface composition of alloy particles. [less ▲]

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See detailHighly dispersed iron xerogel catalysts for p-nitrophenol degradation by photo-Fenton effects
Mahy, Julien ULg; Tasseroul, Ludivine ULg; Zubiaur, Anthony ULg et al

in Microporous and Mesoporous Materials (2014), 197

Several iron xerogel catalysts were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ... [more ▼]

Several iron xerogel catalysts were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ions. The EDAS/TEOS ratio strongly influences the texture of xerogel catalysts. The specific surface area and the micro- and mesoporous volume increase with this ratio. It seems that EDAS plays a nucleating agent role for silica particles and allows to anchor Fe-based moieties inside the silica network. Iron oxide nanoparticles of diameter 1-1.5 nm and Fe3+ ions result, encapsulated in silica particles with sizes of about 10-30 nm in diameter. The iron species was determined by Mössbauer spectroscopy and magnetometry measurements and only Fe3+ species were observed in xerogel catalysts. The Fenton and photo-Fenton effect of these catalysts were evaluated on the degradation of p-nitrophenol in aqueous media under different conditions. Results show that in the presence of H2O2, iron xerogel catalysts present a photo-Fenton effect, reaching 99 % of degradation after 24 h. [less ▲]

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See detailHighly dispersed iron xerogel catalysts for p-nitrophenol degradation by photo-Fenton effects
Mahy, Julien ULg; Tasseroul, Ludivine ULg; Zubiaur, Anthony ULg et al

Poster (2014, July)

Since the beginning of the industrial era, the various human activities have increased steadily, leading to a rapid technological development and a high population growth. Thus, the expansion of the ... [more ▼]

Since the beginning of the industrial era, the various human activities have increased steadily, leading to a rapid technological development and a high population growth. Thus, the expansion of the industry has heavily polluted the atmosphere, soil and water with negative consequences for humans and environment [1]. To decrease this pollution, it exists various treatment methods: chemical, physical and biological [2,3]. Among all these methods, a recent way of treatment is the degradation of pollutants in soils or waters by Fenton and photo-Fenton reactions [3] which use H2O2, iron-based compounds and UV light. In this way, several Fe2O3/SiO2 xerogel catalysts were synthesized by cogelation method by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ions [4]. Five samples were synthesized: four samples with different percentage of iron (0.5, 1, 1.5 and 2.5 theoretical wt% confirmed by ICP-AES measurements), and a sample of pure silica. TEM pictures, nitrogen adsorption-desorption and mercury porosimetry measurements have established that EDAS plays a role of nucleating agent of silica particles [5,6] and allows to anchor iron particles inside silica network [4]. Indeed, it results iron nanoparticles of diameter 1-1.5 nm encapsulated in silica particles with sizes of about 10-30 nm in diameter. The species of iron was determined by Mössbauer spectroscopy and only Fe3+ ions were observed in xerogel catalysts. Then, the Fenton and photo-Fenton effect of these catalysts were evaluated on the degradation of p-nitrophenol (PNP) in aqueous medium in different conditions. Results show that Fe2O3/SiO2 xerogels present a photo-Fenton effect with H2O2, reaching with a sample 99 % of degradation after 24 h. [1] M. A. Khan, A. M. Ghouri, Environmental pollution: its effects on life and its remedies, Journal of Arts, Science & Commerce (Vol. 2), 2011, pg 276-285. [2] M. S. Kuyukina , I. B. Ivshina, Biology of rhodococcus: chapter 9, Springer, 2010, pg 232-256. [3] J. J. Pignatello, E. Oliveros, A. MacKay, Advanced Oxidation Processes for Organic Contaminant Destruction Based on the Fenton Reaction and Related Chemistry, Critical Reviews in Environmental Science and Technology (Vol. 36), 2006, pg 1-84. [4] B. Heinrichs, L. Rebbouh, J.W. Geus, S. Lambert, H.C.L. Abbenhuis, F. Grandjean, G.J. Long, J.-P. Pirard, R.A. van Santen, Iron (III) species dispersed in porous silica through sol-gel chemistry, Journal of Non-Crystalline Solids (Vol. 354), 2008, pg 665-672. [5] S. Lambert, C. Alié, J.-P. Pirard, B. Heinrichs, Study of textural properties and nucleation phenomenon in Pd/SiO2 , Ag/SiO2 and Cu/SiO2 cogelled xerogel catalysts, Journal of Non-Crystalline Solids (Vol. 342), 2004, pg 70-81. [6] B. Heinrichs, S. Lambert , N. Job , J.-P. Pirard, in "Catalyst Preparation: Science and Engineering, J. R. Regalbuto (Ed.)", CRC Press, Taylor & Francis Group, Boca Raton, 2007, p. 163-208. [less ▲]

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See detailRemediation of contaminated soils by the coupled action of microorganisms and metallic oxide nanoparticles
Mahy, Julien ULg; Tasseroul, Ludivine ULg; Masy, Thibaut ULg et al

Poster (2014, March 11)

In this work, it was developed an active "microorganism-nanoparticle" couple for soils bioremediation. The nanoparticles used in this work are iron oxide nanoparticles encapsulated in a silica matrix ... [more ▼]

In this work, it was developed an active "microorganism-nanoparticle" couple for soils bioremediation. The nanoparticles used in this work are iron oxide nanoparticles encapsulated in a silica matrix, called Fe2O3/SiO2 xerogel catalysts. The latter were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS), which is able to form a chelate with iron ions. Characterization of Fe2O3/SiO2 catalysts showed that two parameters strongly influence the gels texture: (i) the EDAS/TEOS molar ratio and (ii) the thermic treatments. The species of iron was determined by Mössbauer spectroscopy and only Fe3+ ions were observed in xerogel catalysts. In parallel, biphenyl degradation tests were achieved in the presence of micro-organisms and different sources of iron (salts or nanoparticles). Tests on the evolution of biphenyl concentration in aqueous medium were also performed alone to determine if the biphenyl undergoes degradation or evaporation in the test conditions. In this way, these tests have identified evaporation and abiotic degradation of biphenyl in the working conditions. Changes of these conditions have been suggested so that in future tests, the degradation of biphenyl by microorganisms and the potential impact of catalysts can be assessed more accurately. [less ▲]

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