J.-N. Foussard

Institut National des Sciences Appliquées de Lyon, Lyons, Rhône-Alpes, France

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Publications (20)42.32 Total impact

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    ABSTRACT: Wastewater originating in the chemical process industries contain high concentrations of organics that must be treated before discharge. Phenol is one of the most important of these pollutants because it is toxic, even at low concentrations. Recently, hydrogen peroxide treatment has emerged as a viable alternative oxidation technique for treatment. It does not form any harmful or intrusive by-products and it is an ecologically clean and non-toxic chemical. However, the methods for treatment of wastewater with hydrogen peroxide are based mostly on homogeneous catalysis by metal ions inducing additional pollution. From this, it was anticipated that the use of heterogeneous catalysis would be a good alternative, thus opening up a new field of investigation. Previous studies, based on screening tests, evidenced the catalytic activity of an MFI zeolite Fe-ZSM-5 for phenol elimination by H2O2. The oxidation tests are carried out in a batch mode, using a stirred glass reactor. The influence of pH, temperature and H2O2 stoichiometric ratio on the phenol oxidation rate with Fe-ZSM-5 is studied. The temperature is below 100°C in order to avoid pressurization of the treatment reactor. Using a H2O2 stoichiometric ratio equal to 1.5 avoids accumulation of any quinone-like by-products. Under these conditions, the catalytic system H2O2 / Fe-ZSM-5 allows a total elimination of phenol and a significant TOC removal (50%) without leaching-off more than 1 ppm of Fe (III) ions. At the end of the reaction period, only carboxylic acids (maleic, fumaric, oxalic, acetic, accumulate. These latter should not be considered as a drawback of this process. The chemical oxidation process would be used only as a detoxification step and such compounds could be treated with a biological process, in a second step.
    Environmental Technology 05/2010; March 1(2000):337-344. · 1.61 Impact Factor
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    ABSTRACT: This paper examines the rate of absorption of molecular oxygen in an aqueous solution of sodium sulphite as a function of temperature over the range of 20–240°C. First, we determined the effect of the various parameters (oxygen partial pressure, sulphite and catalyst concentration, agitation) on the enhancement factor, E. It was observed that an Arrhenius' type relationship could describe the dependence of the physical absorption rate on temperature. According to the degree of agitation, two values for the activation energy: 22.8 and 12.7 kJ · mol−1 are obtained. Our results validate the various models formerly proposed only for the range 10–40°C, but show that they cannot be extrapolated above 50°C. The results also show that a simple test at ambient temperature can be used to predict the oxygen transfer capability of a reactor at temperatures up to 240°C.Afin d'étudier l'influence de la température (20 à 240°C) sur la vitesse d'absorption de l'oxygène moléculaire par une solution aqueuse de sulfite de sodium, nous avons été amenés à préciser l'influence des divers paramètres opératoires sur le facteur d'accélération E. Le domaine de mesure de la vitesse de transfert physique étant déterminé, nous avons observé qu'une équation de type Arrhénius rendait bien compte des résultats expérimentaux. Selon le degré d'agitation, on obtient deux valeurs de l'énergie d'activation: 22.8 et 12.7 kJ · mol−1. Les résultats obtenus dans cette large gamme de température sont en accord avec les divers modèles proposés antérieurement entre 10 et 40°C mais montrent que ceux-ci ne sont pas extrapolables au-delà de 50°C. A la suite de ce travail, il est possible par une simple expérimentation à 20°C de prévoir la capacité oxygénante d'un système jusqu'à 240°C.
    The Canadian Journal of Chemical Engineering 03/2009; 62(4):513 - 520. · 1.00 Impact Factor
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    ABSTRACT: New titanium dioxide (TiO2) based catalysts were prepared by impregnating commercial zeolites in pellets form using a sol–gel technique. Characterization was done with chemical analysis, X-Ray diffraction, scanning electron microscopy, and BET measurements, together with volatile organic compounds (VOC) adsorption equilibrium experiments. TiO2 happened to fix on the inert binder leading to a close intimacy of mixing with the zeolites crystallites, without significant modification of support properties. A diffusion cell was used to produce dilute polluted air streams for dynamic experiments, in which adsorption and photodegradation phases were alternatively carried out. Regeneration of adsorbent was evaluated regarding experimental conditions. Through a comparison with the results obtained on impregnated mesoporous borosilicate beads, it was clarified that zeolite supports had no effect on 1-butanol (BuOH) photooxidation mechanisms. Yet, evidence for mass transfer limitation was found, and attributed to intracrystalline diffusion in zeolites.
    Chemical Engineering Science 01/2003; · 2.61 Impact Factor
  • P. Monneyron, S. Mathé, M.-H. Manero, J.-N. Foussard
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    ABSTRACT: Aiming at regenerating adsorbents, the reactivity toward ozone of two high silica zeolites (HSZ), a dealuminated faujasite Y (Fau Y) and a silicalite (Sil Z), was investigated. In case of Fau Y, no physical adsorption occurred but a total degradation of ozone. This phenomenon was attributed to an active sites-role of silanol groups (SiOH), mainly developed by the dealumination step. In contrast, the ozone adsorption in the smaller channels of Sil Z was important (about 17 mmol g−1), but when a certain local concentration of ozone was reached, the ozone degradation became significant and increased up to 100%. The ozonated zeolites were regenerated in an oven. Whereas the regeneration was total at 773K, a treatment at 500K seemed insufficient since a co-adsorption phenomenon was observed with suspected nitrous oxides (NO2) as a product of ambient nitrogen oxidation. Whereas the Fau Y was not affected at all by ozonation, the adsorption capacities of Sil Z zeolite were enhanced, and it exhibited a higher selectivity for polar compound. This was attributed to a surface modification, by highly reactive species generated during molecular ozone decomposition.
    Chemical Engineering Research & Design - CHEM ENG RES DES. 01/2003; 81(9):1193-1198.
  • P. Monneyron, M.-H. Manero, J.-N. Foussard
    Adsorption Science and Technology - The Third Pacific Basin Conference; 01/2003
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    S Brosillon, M H Manero, J N Foussard
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    ABSTRACT: From experimental results of adsorption of volatile organic compounds (VOCs) on zeolite, we propose simulations of the breakthrough curves based on the Linear Driving Force model. Experiments were run on fixed beds of hydrophobic commercial zeolites. Pollutants chosen are from several chemical classes with different polarities. A good agreement between experimental and numerical results is found when an adjustable value of the internal mass-transfer coefficient is used. A constant value of effective diffusivity is found independent of the nature and the amount of VOCs adsorbed. A relation linking intrapellet mass-transfer coefficient and equilibrium constant is proposed, including the average effective diffusivity, to make predictions of breakthrough curves for any kind of volatile organic pollutant in gaseous effluents.
    Environmental Science and Technology 10/2001; 35(17):3571-5. · 5.48 Impact Factor
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    ABSTRACT: Wet oxidation in subcritical conditions is a new alternative to usual routes for sewage sludge treatment and it complies with environmental standards. The paper presents tests carried out on a batch reactor and on a continuous pilot unit, treating municipal sewage sludge. A method is proposed that shows that the oxidation efficiency in a continuous reactor can only be easily predicted from the residence time distribution and batch tests results. Nevertheless, a partial settling of the solid residue in the continuous bubble column reactor is evident, and it increases the solid residence time and then decreases its organic content with respect to a similar batch test. In addition, these results highlight the considerable influence of temperature in the oxidation reactor and of the type of sewage sludge which is treated. At temperatures around 240 degrees C, foaming can seriously impair the operation of the continuous reactor, because of the presence of non-degraded fatty compounds and surfactants. Moreover, the COD reduction is limited to 70%. On the contrary, at 300 degrees C, COD removal efficiency greater than 80% is achieved without any catalyst additive and, in addition, only highly biodegradable compounds remain in the oxidised liquor.
    Water Science & Technology 02/2001; 44(5):161-9. · 1.10 Impact Factor
  • Brosillon S, Manero M-H, Foussard J.N
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    ABSTRACT: In the present study, co-adsorption of gaseous n-heptane and acetone is studied. The adsorbent is a commercial hydrophobic zeolite. Breakthrough curves and isotherms are measured for three different acetone/heptane mixture ratios and for pure components. Zeolites showed a greater adsorption capacity for acetone alone than for heptane alone. For the mixtures, the majority component was the most adsorbed. Zeolites have a good selectivity for acetone even though acetone is more volatile than heptane. Specific adsorption sites are reserved for acetone adsorption and are not accessible to heptane. The polarity of a component leads to electrostatic interactions with cation exchange. On non-specific adsorption sites, acetone can be displaced by heptane, which is less volatile. Moreover, experiments show that selectivity depends on the ratio of the mixture. For co-adsorption of a mixture of polar and non-polar components, selectivity depends on relative polarity, mixture ratio, and boiling point.
    Environmental Technology 03/2000; 21(4):457-465. · 1.61 Impact Factor
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    Hubert Debellefontaine, Jean Noël Foussard
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    ABSTRACT: Aqueous wastes containing organic pollutants can be efficiently treated by wet air oxidation (WAO), i.e. oxidation (or combustion) by molecular oxygen in the liquid phase, at high temperature (200–325°C) and pressure (up to 175 bar). This method is suited to the elimination of special aqueous wastes from the chemical industry as well as to the treatment of domestic sludge. It is an enclosed process, with a limited interaction with the environment, as opposed to incineration. Usually, the operating cost is lower than 95 Euro m−3 and the preferred COD load ranges from 10 to 80 kg m−3. Only a handful of industrial reactors are in operation world-wide, mainly because of the high capital investment they require. This paper reviews the major results obtained with the WAO process and assesses its field of possible application to industrial wastes. In addition, as only a very few studies have been devoted to the scientific design of such reactors (bubble columns), what needs to be known for this scientific design is discussed. At present, a computer program aimed at determining the performance of a wet air oxidation reactor depending on the various operating parameters has been implemented at the laboratory. Some typical results are presented, pointing out the most important parameters and the specific behavior of these units.
    Waste Management 01/2000; · 3.16 Impact Factor
  • G Deiber, J N Foussard, H Debellefontaine
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    ABSTRACT: Aqueous wastes containing organic pollutants can be efficiently treated by wet air oxidation (WAO), i.e. oxidation by molecular oxygen in the liquid phase, under high temperature (200-325 degrees C) and pressure (up to 150 bar). However, organic nitrogen can be relatively resistant to oxidation and can be harmful to the environment. In the course of treatment, organic nitrogen (N-Org) is converted into ammonia (NH(3)), while organic carbon (C-Org) is converted mainly into carbon dioxide (CO(2)). This can be done without catalysts. In the presence of Mn/Ce composite oxides, it is possible to transform ammonia into molecular nitrogen at a temperature close to 260 degrees C. The direct conversion of organic nitrogen into molecular nitrogen also can be achieved using the same catalyst. This paper discusses the results obtained during the treatment of nitrogenous compounds like aniline, nitrophenol, beta-alanine and ammonia. Laboratory investigations were conducted in a stirred batch reactor with Mn/Ce composite oxides as catalysts. Very limited amounts of nitrites and nitrates were observed with amines, but more significant quantities were found with nitro-compounds. The kinetics of oxidation of ammonia, organic compounds, and more particularly aniline, were investigated. The treatment of a real waste (process wastewater) was also investigated. The dependence of the transformation rate on various parameters (amount of catalyst, temperature, etc.) was established. The rates of oxidation are described by first-order kinetic laws with respect to the various nitrogen species (aniline, NH(3)). Several parallel pathways are considered for the transformation of organic nitrogen, amongst which is an interaction with the catalyst surface. The orders with respect to oxygen and catalyst are established.
    Environmental Pollution 02/1997; 96(3):311-9. · 3.73 Impact Factor
  • Quaternary Science Reviews 01/1997; 16(7). · 4.57 Impact Factor
  • Quaternary Science Reviews 01/1997; 16(7). · 4.57 Impact Factor
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    ABSTRACT: This paper presents an original approach to the treatment of phenolic aqueous wastes using H2O2 with Fe-ZSM-5 as a heterogeneous catalyst. The Fe-ZSM-5 zeolite with MFI structure allows a total elimination of phenol and a significant total organic carbon (TOC) removal at 90°C and atmospheric pressure in a batch reactor. The studies with this Fe-ZSM-5 catalyst deal mainly with the influence of external diffusion and pH on the oxidation process. It appears that the phenol degradation and the toxicity reduction, on the one hand, and the leaching-off of Fe(III) ions in the solution, on the other hand, depend strongly on the pH . In these conditions, an optimwn value exists at pH = 5. At higher pH values, the system becomes less effective. At lower values, a significant leaching-off will induce homogeneous catalysis and the degradation of the catalyst. Generally speaking, when this heterogeneous catalyst is used in the presence of H2O2, the reaction rates depend on the degree of hydroxylation of the aromatic compound incontact with the catalyst. So, a chain radical mechanism could be envisaged.
    Water Science & Technology 01/1997; 35(4):103-110. · 1.10 Impact Factor
  • G. Deiber, J.N. Foussard, H. Debellefontaine
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    ABSTRACT: Aqueous wastes containing organic pollutants can be efficiently treated by wet air oxidation (WAO), i.e. oxidation by molecular oxygen in the liquid phase, under high temperature (200–325°C) and pressure (up to 150 bar). However, organic nitrogen can be relatively resistant to oxidation and can be harmful to the environment. In the course of treatment, organic nitrogen (N-Org) is converted into ammonia (NH3), while organic carbon (C-Org) is converted mainly into carbon dioxide (CO2). This can be done without catalysts. In the presence of composite oxides, it is possible to transform ammonia into molecular nitrogen at a temperature close to 260°C. The direct conversion of organic nitrogen into molecular nitrogen also can be achieved using the same catalyst. This paper discusses the results obtained during the treatment of nitrogenous compounds like aniline, nitrophenol, β-alanine and ammonia. Laboratory investigations were conducted in a stirred batch reactor with composite oxides as catalysts. Very limited amounts of nitrites and nitrates were observed with amines, but more significant quantities were found with nitro-compounds. The kinetics of oxidation of ammonia, organic compounds, and more particularly aniline, were investigated. The treatment of a real waste (process wastewater) was also investigated. The dependence of the transformation rate on various parameters (amount of catalyst, temperature, etc.) was established. The rates of oxidation are described by first-order kinetic laws with respect to the various nitrogen species (aniline, NH3). Several parallel pathways are considered for the transformation of organic nitrogen, amongst which is an interaction with the catalyst surface. The orders with respect to oxygen and catalyst are established.RésuméLe procédé d'oxydation en voie humide (WAO) a montré son efficacité lors du traitement des effluents organiques aqueux industriels. L'oxydation s'effectue en présence d'oxygène moléculaire à haute température (200–325°C), en phase liquide, et donc à haute pression (jusqu'à 150 bar). Cependant, les composés organo-azotés peuvent s'avérer résistants au traitement par oxydation et s'avèrent quelquefois toxiques pour l'environnement. Lors du traitement dans des conditions classiques, c'est-à-dire sans catalyseur, l'azote organique (N-Org) est transformé en ammoniaque (NH3) alors que le carbone organique (C-Org) est oxydé, principalement en dioxyde de carbone (CO2). A l'inverse, l'utilisation d'un catalyseur tel que l'oxyde mixte permet, à une température de l'ordre de 260°C, de transformer l'azote ammoniacal (NH3) en azote moléculaire (N2). Ce même catalyseur permet aussi la converson directe de l'azote organique (N-Org) en azote moléculaire (N2). Cet article rend compte de résultats obtenus lors du traitement d'effluents synthétiques contenant des composés tels que l'aniline, le nitrophénol, la β-alanine et l'ammoniaque. Les essais ont été conduits en réacteur autoclav̊e discontinu, en présence du catalyseur dont les caractéristiques sont indiquées dans le tableau 1. En l'absence de catalyseur, les tableaux 2 et 6 mettent en évidence que la transformation en ammoniaque est possible, mais que la transformation en azote moléculaire n'est jamais obtenue. Les tableaux 3 et 6 établissent qu'en présence de catalyseur, seules de très petites quantités de nitrites et nitrates sont habituellement obtenues, en comparaison de l'azote moléculaire formé. Dans le cas du composé nitré, des quantités plus significatives peuvent apparaître. Une étude cinétique a montré que la réaction est d'ordre 1 par rapport à l'ammoniaque (équation 3, tableau 4 et figure 2). De façon similaire, l'étude cinétique de l'oxydation de composés organiques a permis de proposer une loi de vitesse qui découle de l'hypothèse de réactions parallèles et/ou successives, dont une interaction avec la surface catalytique, conformément à la réaction II et aux équations 4 et 5. Le schéma réactionnel admet que l'ensemble de ces réactions est d'ordre 1 par rapport à l'espèce azotée. Les figures 5 et 6 et les figures 7–10 permettent de comparer les résultats expérimentaux et les courbes modèles correspondant aux équations 4 et 5. Les tableaux 7 et 8 listent les valeurs des différents paramètres retenus après ajustement. Un essai de traitement d'un effluent organo-azoté réel (eau de procédé) est présenté dans les tableaux 9 et 10 et sur la figure 11.
    Environmental Pollution 01/1997; · 3.73 Impact Factor
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    ABSTRACT: Aqueous wastes containing organic pollutants can be efficiently treated by wet air oxidation (WAO), i.e. oxidation by molecular oxygen in the liquid phase, under high temperature (200 to 325°C) and pressure (up to 150 bar). In western Europe, only an handful of industrial plants are in operation. Most of them were designed by extrapolating results from pilot plants. Only a very few studies have been devoted to the scientific design of such reactors (bubble columns). This paper discusses what needs to be known for this scientific design. The usual design methods assume that the column is divided into a number of cells. Each cell is a perfectly mixed reactor connected with the contiguous cells. Reliable data and models are available for hydrodynamics (axial dispersion, gas hold up) and mass transfer. Data are also needed for the kinetics of chemical reactions and are available from numerous sources, but have not yet been generalised. The thermodynamics (fugacities and enthalpy) ofthe gas phase can be determined with the Peng Robinson equation of state, and the Henry law for the solubility of gases in water describes the equilibrium conditions. But additional data are needed for water solutions containing salts. This paper describes a method that allows such a determination to be made by establishing rigorous balances on a batch autoclave. At present, these data are being used to implement a computer program aimed at determining the performance of a wet air oxidation reactor depending on the various operating parameters. Some typical profiles within the reactor are presented, establishing that the pH of the solution is a very important parameter.
    Water Science & Technology 01/1997; 35(4):111-118. · 1.10 Impact Factor
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    ABSTRACT: There is growing concern about the problems of waste elimination. We should consider our environment as being borrowed from future generations and refrain from leaving a legacy of problems we are not able to solve. Various oxidation techniques are suited for the elimination of organic aqueous wastes, but because of the environmental drawbacks of incineration, enclosed processes, like liquid phase oxidation should be preferred. Wet air oxidation (WAO) under high temperature (200-325 degrees C) and pressure (50-150 bar) is suited to such liquid wastes and various catalysts, including hydrogen peroxide, can be used in order to increase the efficiency without increasing temperature and pressure. Wet Peroxide Oxidation (WPO) is a similar process. A comparable oxidation efficiency is obtained when using hydrogen peroxide as the oxidising agent instead of oxygen, at a temperature of only 100-120 degrees C. As opposed to WAO, which is capital intensive, WPO needs limited capital but generates higher running costs. The paper reviews the major results obtained for both processes and assesses the field of possible application of each of them. TOC removal efficiencies typically obtained range from 65 to 90% or more for most of the pollutants.
    Environmental Pollution 02/1996; 92(2):155-64. · 3.73 Impact Factor
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    ABSTRACT: Wet Air Oxidation (WAO), i.e. oxidation by molecular oxygen achieved in a liquid phase under high temperature (up to 300°C) and high pressure (up to 100 bar), has been widely studied in order to convert organic pollutants into carbon dioxide. This paper is a contribution to the treatment of organic pollutants containing nitrogenous compounds by wet air oxidation. These nitrogenous compounds can be converted into molecular nitrogen, absolutely harmless for the environment. The use of hydrogen peroxide, associated with ferrous salts promotes the formation of oxidising radicals and is shown to be an efficient technique for allowing the process to be efficient under less drastic conditions (around 200°C). It is shown that such a technique converts, in a first step, the organic nitrogen mainly into ammonia. The second step is the conversion of ammonia into molecular nitrogen. It is established that this is possible to obtain when using Mn/Ce composite oxide as a catalyst at a temperature close from 260°C. The paper considers also the coupling of the two steps and the direct conversion of organic nitrogen into molecular nitrogen, that can be achieved when using the same catalyst as hereon.
    Environmental Technology 06/1995; 16(7):645-655. · 1.61 Impact Factor
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    ABSTRACT: The wet peroxide oxidation process (WPO®) which was developed at the laboratory uses the Fenton's reagent at high temperature. But the reaction efficiency is limited by the accumulation of volatile fatty acids such as oxalic, malonic, succinic and acetic acids (hereafter OMSA). In order to improve the efficiency of the original process, different transition metal ions are tested as catalyst. The experimental results indicate that the system using homogeneous Fe, Cu, and Mn is a promising one. The oxidation of carboxylic acids is quite completed under mild working conditions (T < 100°C, pH = 3, p = 1 atm, reaction time = 1 h, stoichiometric quantity of H2O2 = 1.5). Optimal design methodology is applied to the catalytic mixture Fe:Cu:Mn in order to determine the optimal proportions of each metal. This results in the determination of an important synergistic effect between the metals and an optimal zone. Cu(II), Mn(II) or Fe(II) alone have a slight catalytic effect while the association is very effective on the oxidation of the mixture of carboxylic acids (OMSA). This apparent synergetic effect existing among them can be explained by the main specific roles of Cu(II) and Mn(II) ions. They respectively enhance significantly the oxidation rate of acetic and oxalic acids.
    Environmental Technology 06/1995; 16(6):501-513. · 1.61 Impact Factor
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    ABSTRACT: The wet air oxidation (WAO) process catalysed by hydrogen peroxide coupled with bioxidation for the treatment of olive mill wastewaters (OMW) was investigated. OMW cannot be conveniently treated by biological processes as they contain important amounts of phenol‐like compounds, toxic and recalcitrant to biodegradation. Oxidation was conducted according to the “hydrogen peroxide promoted wet air oxidation”; process between 180 and 200 ˆC. It consists of injecting continuously hydrogen peroxide at a low dosage (10% on a COD basis) into a WAO reactor in order to promote the radical reactions and then lowering the temperature and pressure constraints. WAO treatment allows a complete decolouration of the solution, a 77% chemical oxygen demand (COD) reduction; the remaining COD is mainly low molecular weight carboxylic acids (chiefly acetic) easy for a biological post‐treatment. Compared to the various processes reported in the literature, this two step process offers a good opportunity for OMW depollution.
    Environmental Technology - ENVIRON TECHNOL. 01/1994; 15(4):323-332.
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    ABSTRACT: ChemInform is a weekly Abstracting Service, delivering concise information at a glance that was extracted from about 100 leading journals. To access a ChemInform Abstract of an article which was published elsewhere, please select a “Full Text” option. The original article is trackable via the “References” option.
    ChemInform 01/1991; 22(15):292-292.