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Mathematics and Natural Science MATHEMATICS AND NATURAL SCIENCE Proceedings of the Third International Scientific Conference – FMNS2009 3 – 7 June 2009 Faculty of Mathematics and Natural Science VOLUME 1 South-West University “Neofit Rilski” Blagoevgrad Third International Scientific Conference – FMNS2009 South-West University, Faculty of Mathematics and Natural Science 3 – 7 June 2009 ORGANIZING COMMITTEE: Honorary Chairman: Prof. Ivan Mircev, PhD, Rector of the SOUTH-WEST UNIVERSITY "NEOFIT RILSKI" Chairman: Assoc. Prof. Borislav Yurukov, PhD, Dean of the Faculty of Mathematics&Natural Sciences Prof. C. Cankov (Bulgaria) Members: Prof. Iv. Ganchev (Bulgaria) Prof. Ilia Giudjenov, PhD Prof. S. Grozdev (Bulgaria) Assoc. Prof. Stanko Shtrakov, PhD Prof. D. Havlichek (Czech republic) Assoc. Prof. Mitko Stoev, PhD Prof. Ken Y. Hsu (Taiwan) Assoc. Prof. Luben Mihov, PhD Prof. G.-J. Krauss (Germany) Assoc. Prof. Stefan Manev, PhD Prof. C. Milkova (Bulgaria) Assoc. Prof. Mihail Mihailov, PhD Prof. T. Pavlovich (Serbia) Assoc. Prof. Valentin Hristov, PhD Prof. D. Tsipas (Greece) Assoc. Prof. Stefan Stefanov, PhD Dr. eng. A. Majchrzycka (Poland) Assist. Prof. Ivan Trenchev, PhD Assist. Prof. Grigor Iliev Revewers: Prof. Tsenka Milkova Assoc. Prof. Stefan Stefanov PROGRAM COMMITTEE: Assoc. Prof. Penka Bozarova Assoc. Prof. Stanko Shtrakov Assoc. Prof.Valentin Hristov Chairman: Prof. Kiril Chimev, DrSc Assoc. Prof. Luben Mihov Members: Assoc. Prof.Ivan Drenovski Acad. P. Bonchev (Bulgaria) Assoc. Prof.Michail Michailov Acad. K. Boyanov (Bulgaria) Assoc. Prof.Plamen Gramatikov Acad. Evg. Golovinski (Bulgaria) Assoc. Prof.Boyko Kolev Acad. T. Nikolov (Bulgaria) Assoc. Prof. Stefan Manev Acad. St. Dodunekov (Bulgaria) Assoc. Prof. Krasimir Stoyatoyanov Acad. Al. Popov (Bulgaria) Corr. Member of BAS J. Stamenov Prof. A. Antonov (Bulgaria) Prof. P. Argyrakis (Greece) Prof. P. Frangos (Greece) Prof. A. Borisov (Bulgaria) Third International conference FMNS2009 – Faculty of Mathematics and Natural Science A Novel Approach to the Fuel Cell Technology Mario Mitov1, Rashko Rashkov2, Stoyan Hrsitov3, Anastasia Kaisheva3 1- Department of Chemistry, South-West University, Blagoevgrad, Bulgaria 2- Institute of Physical Chemistry – BAS, Sofia, Bulgaria 3- Institute of Electrochemistry and Energy Systems – BAS, Sofia, Bulgaria Abstract: In this paper, results from implementation the first year pro- gram of a project “Metal Hydride – Air Cell” are presented and discussed. Conventional and newly synthesized materials have been studied as anode and cathode electrocatalysts for borohydride oxidation and oxygen reduc- tion reactions, respectively. Initial tests with experimental fuel cell were also conducted. Based on analysis of results, some of studied materials are pro- posed for further investigations during next stages of the project. Keywords: metal hydride electrodes, alkaline borohydrides, electrooxi- dation, air gas-diffusion electrodes, Direct Borohydride Fuel Cell. 1. INTRODUCTION A new generation of devices and technologies aiming to overcome the disadvantages of existing energy system is under intensive research and development. Among the most perspective technologies is that of fuel cells [1-3]. These are electrochemical devices that convert the energy of chemical re- actions similar to combustion processes into electricity. The mostly developed types are fuel cells using hydrogen as a fuel. However, various problems connected with technologies for hydrogen pro- duction, storage and transportation, as well as use of expensive electrocata- lysts and, in some cases, electrolytes, exist and should be overcome for commercialization of the technology. Although hydrogen is the fuel of choice, other hydrogen-rich compounds such as alkaline hydrides, borohydrides, alanates, etc. are also of interest [4,5]. Sodium borohydride is one of the most intensively investigated among other hydrides. Besides high hydrogen content among its advantages are it high solubility in water, easy stabilization by addition of alkaline base, con- trollable generation of hydrogen by catalyzed hydrolysis reaction: - - (1) BH 4 + 2H2O → BO 2 + 4H2 The formed borates are environmental safety and can be regenerated. 3 Section: “Chemistry” In addition, sodium borohydride can undergo electrochemical oxidation via following reaction: - - - - (2) BH4 + 8OH Æ BO 2 + 6H2O +8e The big number of participating electrons as well as highly negative po- tential of above reaction makes it very useful for practical application in electrochemical power sources. However, proper electrocatalysts are re- quired for the effective borohydride oxidation. Two important applications can be realized based on upper discussed reactions - hydrogen-on-demand (HOD) generators [6] and Direct Boro- hydride Fuel Cells (DBFC) [5,7]. Based on our previous experience in the fields of metal hydride and air gas-diffusion electrodes [8,9], we have started a project aiming at develop- ment of metal hydride – air fuel cell, using sodium borohydride as a fuel. In this paper, we summarize some of major results obtained during the first year of the project. 2. EXPERIMENTAL 2.1. Materials and reagents Two types of materials have been principally studied as potential anode materials for direct borohydride oxidation – commercial metal hydride alloys and newly synthesized Co-based hydrogen-absorbing nanocomposite elec- trodeposits. Except conventional Co-Ni and СоТМРР catalysts, other multicompo- nent systems (NiCoMnB, NiWTiOx, NiMoW) have been obtained by electrodeposition for testing as catalysts for air gas-diffusion electrodes. Several plastics have been chosen for construction of experimental fuel cell – PVC, PMMA and polycarbonat Macrolon®. Chemical resistance in concentrated base solutions, wide temperature range operation (up to 80- 100 oC), transperancy, etc. were among the leading criteria for chosing these materials. Various separators and membranes as polyethylene separators DA- RAMIC®, plastic separators DARAK®, cellulose separators ARMORIB®, Na- fion™ membranes, etc. have been tested for effective separation of the ano- lyte and catholyte in the experimental cell. Sodium borohydride (purum p.a., Fluka) was used for preparation of the anolyte. Potassium or sodium hydroxide solutions were used as alkaline media. 2.2. Electrodes Different technologies have been used for preparation of electrode samples. Third International conference FMNS2009 – Faculty of Mathematics and Natural Science Electrodes for borohydride electrooxidation were produced by following methods: Pre-determined amount of a metal hydride alloy was mixed at various proportions with additives for increasing conductivity (nickel powder, gra- phite or VULCAN 72 hydrophobized carbon black) and binding agent (PTFE emulsion, PTFE paste or polyvinyl alcohol solution). After homogenization, the mixture was cold- or hot-pressed on Ni-foam. Cobalt-based nanocomposites were directly electrodeposited on Ni- mesh or Ni-foam and pressed after that. Air gas-diffusion cathodes were made in a following way: Double layer tablets, comprising a porous hydrophobic gas layer made off a carbon material, modified by PTFE, and a catalytic layer made from a mixture of the same hydrophobic material and porous catalyst [10], were pressed on the both sides of Ni-mesh, used as a current collector, at 200 kg/cm2 and 280о С for 2 minutes. 2.3. Methods A set of electrochemical methods has been used for characterization of electrode performance in borohydride solutions. The tested electrodes were polarized anodically in base-stabilized so- dium borohydride solutions at varying constant currents. Simultaneously, the kinetics of hydrogen evolution due to borohydride hydrolysis was moni- tored by means of water displacement method [11]. In other set of experiments, galvanostatic discharge curves were taken with the same electrodes in stabilized borohydride electrolytes and in 6M KOH electrolyte after overnight immersion of electrodes in borohydride – containing solution. The electrochemical experiments were carried out in a specially con- structed hermetic water-jacketed three-electrode cell with an outlet for gen- erated gases. The tests were performed using PJT 35-2 potentiostat- galvanostat (Radiometer Tacussel) with IMT 101 electrochemical interface and Volta Master 2 software. Steady-state polarization characteristics of investigated air gas-diffusion electrodes were obtained when operating with air or with pure oxygen in strong KOH electrolyte, using a half-cell arrangement. The potentials of air electrodes were measured against Zn reference electrode. Volt-ampere characteristics of an experimental two-electrode metal hy- dride-air cell were taken using varying resistances. Metal hydride electrode prepared from commercial AB5-type alloy and air gas-diffusion electrode with CoTMPP catalyst were used as an anode and a cathode, respectively. The geometric area of both electrodes was 6 cm2. The anode and cathode compartments were separated by DARAMIC® separator, pre-treated with Nafion 117 (Fluka). Borohydride-containing 6M KOH electrolytes were used 5 Section: “Chemistry” as an anolyte and the cathode compartment was filled with 6M KOH solu- tion. 3. RESULTS AND DISCUSSION 3.1. Studying of “metal hydride electrode – borohydride electrolyte” system Anodic polarization curves, obtained with metal hydride electrodes in stabi- lized borohydride solution, are presented on figure 1: -1200 -1100 CoNiMnB -1000 -900 AB5 E, mV (vs.H/HgO) mV E, -800 -700 0 50 100 150 200 i, mA/cm2 Fig. 1: Polarization curves obtained
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