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Kinetic Study of the Dissolution of Vanadyl Sulfate and Vanadium

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Kinetic Study of the Dissolution of Vanadyl Sulfate and Vanadium Kinetic study of the dissolution of vanadyl sulfate and vanadium pentoxide in sulfuric acid aqueous solution Ranine El Hage, Fabien Chauvet, Béatrice Biscans, Laurent Cassayre, L. Maurice, Théodore Tzedakis To cite this version: Ranine El Hage, Fabien Chauvet, Béatrice Biscans, Laurent Cassayre, L. Maurice, et al.. Kinetic study of the dissolution of vanadyl sulfate and vanadium pentoxide in sulfuric acid aqueous solution. Chemical Engineering Science, Elsevier, 2019, 199, pp.123-136. 10.1016/j.ces.2019.01.024. hal- 02290658 HAL Id: hal-02290658 https://hal.archives-ouvertes.fr/hal-02290658 Submitted on 17 Sep 2019 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. OATAO is an open access repository that collects the work of Toulouse researchers and makes it freely available over the web where possible This is an author’s version published in: http://oatao.univ-toulouse.fr/24225 Official URL: https://doi.org/10.1016/j.ces.2019.01.024 To cite this version: El Hage, Ranine and Chauvet, Fabien and Biscans, Béatrice and Cassayre, Laurent and Maurice, L. and Tzedakis, Théo Kinetic study of the dissolution of vanadyl sulfate and vanadium pentoxide in sulfuric acid aqueous solution. (2019) Chemical Engineering Science, 199. 123-136. ISSN 0009-2509 Any correspondence concerning this service should be sent to the repository administrator: [email protected] Kinetic study of the dissolution of vanadyl sulfate and vanadium pentoxide in sulfuric acid aqueous solution a a b c a R. El Hage , F. Chauvet , B. Biscans b, L Cassayre , L. Maurice , T. Tzedakis ,* • Laboratoirede Génie Chimique, UMR CNRS 5503, CAMPUS Université Toulouse 111 - Paul Sabotier,FSI. 118, Route de Narbonne, 31062 Toulouse,France • Laboratoirede Génie Chimique, UMR CNRS 5503, CAMPUS/NP - ENSJAŒT, 4 allée Emile Manso, 31 432 Toulouse,France < UniversitéToulouse 111 - PaulSabotier, 118, Route de Narbonne, 31062 Toulouse, France HIGHLIGHTS • Vanadium(IV) sulfate VOS04 and vanadium (V) pentoxide V2 05 dissolution . • Temporal evolution of the concentrations of vo2• and VOi• at various temperatures. • Understanding the dissolution limitations: vrv -+mass transfer; vv -+ reaction with W. • Simple kinetic models to predict the evolution of vü2•and V02• concentrations. ARTICLE INFO ABSTRACT Keywords: The study deals with the 'vanadium (IV) sulfate' and 'vanadium (V) pentoxide' dissolution processesin 2 Vanadyl sulfate 3 M H2S0 4 aqueous media. Severa( measurements of the concentration of dissolved vo • and VOi were Vanadium pentoxide achieved in the range of O 40 •c, and allowed to understand thelimitations of the dissolution process Dissolution kinetics ('endothermic' mass transport for V0S04 and 'exothermic' reactionwith the proton for V205 ). ln addi Vanadium redox battery lion, simple models were proposed (diffusion/accumulation for V0S0 and kinetic rate for V 0 ) and their Solubility 4 2 5 resolution leads to theoretical kinetic equations describing the temporal evolution of these concentra lions with satisfactory agreement with the experimental curves. Solubility's data and their temperature dependence were determined for both vanadium compounds involved 1. Introduction vanadium" redox tlow battery (VRFB) developed in the 1980's by Rychcik and Skyllas Kazacos (1988), Skyllas Kazacos et al. (1988) Renewable energy storage studies have expanded in the past and has been widely explored since (Cunha et al., 2015; Skyllas decades due to the rapid increase in energy consurnption, limited Kazacos et al., 2016, 2015, 2013). fossil fuels reserves and growing ecological concems of their The battery was introduced to overcome the problem of cross impact on health and environment. contamination of electrolytes, inducing capacity lasses reported Only a very limited number of systems enable energy storage primarily by NASA researches in the 1970s for the Fe Cr system such as thermal storage, pumped hydropower and compressed (Thaller, 1977, 1974). Given that the same element in different oxi air energy storage (Amirante et al., 201 7; Ding et al., 2009). Electro dation states is used in both compartments of the VRFB, no con chemical storage constitutes an interesting alternative and tamination of the active material will occur in case ions cross the recently the Redox Flow Battery (RFB) acquired a great importance ionic separator. The redox couples employed are v<111l/'.f11l and as they have the particularity of converting and storing energy by y{Vl/y{ 111l for the negative and the positive half cells respectively using electroactivespecies dissolved in electrolyte solutions (Wang (Sum et al., 1985; Sum and Skyllas Kazacos, 1985), and the only et al., 2013; Leung et al., 2012). The most spread RFB is the "ail redox reactions involved are thus the valence changes ofthe vana dium ions. The electrolyte solutions are usually prepared in 2 3 M * Corresponding author at: Chemical Engineering Laboratory, UMR CNRS 5503, sulfuric acid, even if other electrolytes have been investigated FSL Université Toulouse Ill - Paul Sabatier, 118, Route de Narbonne. 31062 (generation 2 and 3 of the VRB) (Skyllas Kazacos et al., 2007. The Toulouse,France. VRB is characterized by a long life span (>10,000 cycles) (Ashby E-mail address: [email protected](T. Tzedakis). and Polyblank, 2012), low maintenance cost and deep discharge https://doi.org/10.1016/j.ces2019.01 .024 Nomenclature A(765 nm) absorbance at the wave length of 765 nm PES polyether sulfone A Arrhenius pre exponential factor R° initial radius of the particle (m) aVOSO4 solid activity of the solid compound R(t) radius of the particle at the dissolution time t (m) a constant (Leveque correlation) r initial reaction rate (mol L 1 s 1) A1,A2,A3 and A4 constants (defined in Appendix A) rglobal total rate of the reaction of the dissolution of V2O5 (mol 2+ 1 1 Cbulk concentration of VO in the bulk (M) L s ) 2+ Csurface Csaturation superficial concentration of VO , assumed at RFB Redox Flow Battery dp Âu À q saturation (M) Re Reynolds number m dp  u  l dp particle diameter at time t (lm) SEM scanning electron microscope D diffusion coefficient (m2/s) S surface of particles involved in the dissolution process 2 Ea activation energy (J/mol) (m ) eðÞt thickness of the spherical crown film, function of the Sc Schmidt number = m/D  time (m) Sh Sherwood number (Sh kðtÞ dp = = D e absorptivity (cm 1 M 1) 2 þ a  Re1 2  Sc1 3 ! Leveque correlationÞ DRH reaction enthalpy (J/mol) t dissolution time (expressed in ‘s’ for VOSO4 and in ‘h’ for j number of iterations taken as 100 V2O5) À k kinetic constant following the Arrhenius law (unit func u average rate of the liquid around the solid particle cal tion of the reaction order) culated from the stirring rate (m/s), assumed constant D 2+ kð Þ mass transfer coefficient of the VO around the solid during the experiment time t eð Þ t 1 2 particle of VOSO4 (m s) m kinematic viscosity (m /s) l=q 2+ m moles number of dissolved VOSO4 (to VO ) into the DU internal energy (J/mol) bulk VRFB Vanadium Redox Flow Battery 3 M molar mass of the solid VOSO4 5H2O (kg/mol) V solid volume present in the solution at time t (m ) N number of VOSO4 particles having a certain initial ra V l total volume of the solution (including both the liquid dius R° and the powder) n°(V) initial moles number of V2O5 (mol) x stirring rate (rpm) + n°(H) initial moles number of H (mol) X moles number of V2O5 dissolved at time t q specific gravity of the powder (kg/m3) PTFE polytetrafluoroethylene 2þ 2 capability (Vijayakumar et al., 2013). The energy density of the bat VOSO4ðsÞ ¡ VO +SO4 ð3Þ tery is largely depending on the volume and concentration of the vanadium electrolytic solutions and numerous authors studied ¡ þ 2 ð Þ the effect of the composition of electrolyte solutions (Choi et al., (VO2)2SO4ðsÞ 2VO2 +SO4 4 2017; Skyllas Kazacos et al., 2016) on the performance of the As mentioned by Rahman and Skyllas Kazacos (2009), vana battery. dium (V) can precipitate after 1000 h at 50 °C and the redissolution Despite that, stable solutions with vanadium concentrations of the oxide V2O5 (Rahman, 1998) appears to be difficult. Numer higher than 2 M could not be achieved in the working conditions ous authors (Ivakin and Voronova, 1973; Vijayakumar et al., of the VRB, limiting the quantity of stored energy to around 2011; Kausar, 2002) conducted studies to understand the poor 3 40 kWh/m . thermal stability of V(V) at high temperatures. They showed that The electrolyte in the negative electrode compartment does not the precipitation process of V2O5 is endothermic and thus (III) seem to exhibit major limitations related to the solubility of V enhanced when temperature increases. (II) (II) and V , but one point to mention is that V is easily oxidized Moreover, the aqueous chemistry of vanadium (V), studied by by air (choi et al., 2013). One important limitation encountered several authors (Crans et al., 2004; Elvingson et al., 1998), inferred by the vanadium battery appears to be related to the precipitation the presence of many species as a function of the solution’s pH. It of compounds in the positive electrode: precipitation of the V(IV) at + was suggested that pervanadyl or dioxovanadium cation (VO2)is (V) low temperature and precipitation of the V compounds at high the main species formed in the lower pH range (0.5 1.3) (Baes temperature.
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