Aceh International Journal of Science and Technology. Preliminary Study on Benzoic Acid Adsorption from Crude Active Coals and Bentonite

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Aceh Int. J. Sci. Technol., 5(1 : 38-44 Aceh International Journal of Science and Technology ISSN: 2088-9860 Journal hoepage: http://jurnal.unsyiah.ac.

Bachir, El Bayadh, Algeria. 2 Faculty of science and technology, University Centre, Ain Teouchent, Algeria. 3 Faculty of Science and Technology, University of Djillali liabes, Sidi bel Abbes, Algeria.

1 Aceh Int. J. Sci. Technol., 5(1 : Aceh International Journal of Science and Technology ISSN: Journal hoepage: Preliinary Study on Benzoic Acid Adsorption fro Crude Active Coals and Bentonite Abbes Boucheta 1*, Soufi Kacii 2, Razika Bared 3 1 Faculty of science and technology, University Centre, Nour Bachir, El Bayadh, Algeria. 2 Faculty of science and technology, University Centre, Ain Teouchent, Algeria. 3 Faculty of Science and Technology, University of Djillali liabes, Sidi bel Abbes, Algeria. Corresponding author eail: abbes.hissi@yahoo.fr Received : 26 February 2016 Accepted : 24 Online : 30 Abstract - We studied the adsorption of pollutant benzoic acid by the odified bentonite of Maghnia (west of Algeria, and coal (Coal fro the ines, southwest of Algeria, Bechar area under three fors, crude and activated. Kinetic data show that the balance of bentonite (as aended adsorbs organic acids better than activated and raw coal. Indeed, the intercalation of bentonite with benzoic acid causes an iproveent in the texture of porous aterial, which allows its use in the adsorption of organic copounds. The adsorption isothers (Languir and Freundlich indicate that the adsorption of benzoic acid by the coal and bentonite yielded results favorably. The results obtained showed the practical value of using the activated coal and bentonite (as aended in the field of reediation of water containated with organic pollutants. Keywords: Bentonite; Coal; Adsorption; Benzoic acid; Kinetic Introduction Coal is a sedientary rock of organic origin, which coes fro the degradation of a wide variety of precursor s higher plants, ferns, algae, fungi, spores, etc. Land filling, progressive organic aterial causes their aturation, essentially by increasing the teperature paraeter plus the pressure for ebedded coals. This developent led to Coalification called anthracite and is accopanied by considerable physical and cheical changes (Abbes et al., The geologic age of the carbons is between 300 illion years. The organic aterial is enriched with carbon initially losing water and carbon dioxide, and then the first liquid hydrocarbon and gas. The coal is ainly coposed of carbon, hydrogen, oxygen and a little sulfur and nitrogen. Study of paleogeographic of different geological epochs of Algeria has shown that only the continental forations, the Carboniferous contain indices and deposits of coal having a certain value. In ore recent forations of the Jurassic, Cretaceous and Tertiary lignite few clues. Northern Algeria Paleogeography shows no conditions for the foration of coal. Adsorption techniques have been successful in reoving organic species. Currently, coal is the ost coonly used adsorbent through its adsorbent power which is very iportant against the organic copounds, but the inconvenience is that coal is expensive in costs (Loison et al., 1989 the preparation requires large investents (oxidation, grinding, pyrolysis, activation, packaging. In this context, that we proposed to test adsorbents copetitive with coal-based clays available, in large quantities in our country, because of its easy and inexpensive operation. Clays are regarded today as being interesting adsorbent aterials. Because of their low cost, abundance on all continents, their ion exchange properties and high surface area, the ability of clay inerals (BENTONITE, Montorillonite to adsorb organic olecules and / or ineral is a subject that has aroused great interest for any years (Akçay et al., 2004; Bouras, The objective of the present work was to eliinate of phenol and benzoic acid by adsorption on a carbon raw coal and activated (Coal fro the ine to the Bechar region and bentonite fro the Region Maghnia. The developent of such effective barriers, local resource base can help to partially 38

2 Aceh Int. J. Sci. Technol., 5(1 : solve the proble of water containation. The present work attepts to solve pollution probles in watery surroundings by aroatic copounds such as the phenol and the benzoic acid. Several ways of eliination of these copounds were the object of different (Bared et al., Materials and Methods An Algerian Coal fro the region of Bechar was used as the starting aterial. The characteristics of the adsorbent used are shown in Table 1 (Abbes et al., 2010; Eren et al., The coal coes fro oxidized organic atter or coal fossilized wood. It is the densest aceral (density between 0.4 and 0.8, hard but friable, rich in carbon, hydrogen-poor and volatile atter The inerals are generally low proportion in coal are( Si,Fe,Ca,Al,Mg,K.Na,Al,B,Va,Ta les Matières Minérales Sont constituées D'inclusions Minérales visibles à l'analyse icroscopique. After burning coal, ineral aterials are the ashes (Deul et al., Preparing raw coal and pyrolysis The coal is crushed using an electric grinder (SM 100 Type RETSH Then sifted through 03,502 pulverizes type and brand Fritsch, to be reduced to eleentary particles with a diaeter between 0.13 and These aterials subjected to pyrolysis which consists of a theral activation, calcination at 700 C by controlled theral prograing for 2h (Abbes et al., To achieve pyrolysis equipent ust be cleansed and arrow, then a saple of about 45g of 0.2 diaeter coal is placed in a quartz reactor itself - sae content in a horizontal furnace. A purge is carried out for 15 in with argon. One begins to heat at 1000 o C. The saple was heat-treated in an argon flow 80 c3 / in. The heating rate was 50C / in. The peranence tie at the final teperature is 30 inutes Yields ash coal were deterined, (Graiyna, 1996.Initial ass of crude coal = 45g., ash efficiency=0.8 %, coal efficiency=51 %. Final ass of Coal = 23g.Ash Mass = 0.36g. Pyrolysis of a carbonaceous precursor, oxygen rich, low aroatic, is ade to obtain a solid with high carbon content. The carbon enrichent is done by heat treatent under an inert atosphere. During this process, we see an eliination of volatile aterials: water (resulting fro a reaction of hydration of alcohol groups and carbon dioxide (decarboxylation product or decoposition lactones and anhydride, then onoxide atos which share in general at a higher teperature beyond 550 C (resulting fro the decoposition of aldehydes and ketones, and finally liquid hydrocarbon (such as- tar and volatile gaseous hydrocarbons. Table1. Coal characteristics of the ines in the area of Bechar Hydrogen Nitrogen Sulfur Oxygen Inorganic Carbon Ultiate wt.%, dry ash-free basis Ash Total sulfur Huidity Volatile atter Fixed carbon Organic Carbon Proxiate wt.%, as-received ,97-5,3 0,2-0,8 12,0-24,5 46, Table 2. Analyzes results of trace eleents in coal Analysis eleents Percentage% Analysis eleents Percentage% Si Ni Fe Sn Ca Zn Al Li 0.01 Mg Cu K Sr 0, Na Cd Mn Cr V Sb 0.01 Ba Pb 0.01 Ti

3 Aceh Int. J. Sci. Technol., 5(1 : Cheical activation of coal by ZnCl2, NaOH, H 3 The activation role, reoved all heavy hydrocarbons, tars type which reain fixed in the coal, and it also helps develop pores, thus increasing the surface of the active substance. The calcination reoves volatile aterial in order to keep only the carbon skeleton. 2g coke ixed with a solution containing 10 c 3 of water, and 4 g of active agent, for 2 hours every tie the experient was repeated with three active agents (H 3, ZnCl 2, and NaOH.The saples were dried at (110 C for 24 hours in an oven. The dry ixtures were heat treated, is added a strea of argon (80 c3/in into a horizontal cylindrical oven.the heating rate of 50 C / in and the activation teperature of 700 C for 2H.The activated coal washed with HCl (5M, then with distilled water until chloride ion purification. Finally, the saple was dried at 1100 C for 12 h. Coal efficiency enabled by H 3> NaOH by activated coal efficiency> activated coal yield is ZnCl 2.NaOH by activated coal ash rate> coal ash rate activated by ZnCl 2> Ash content of coal activated by H 3.Phosphoric acid is the best activating agent because of the ash yield of the activated coal H3PO4 is 9%, which a very large value. Table 3. Output of the activated coal Initial Mass 2g Final Mass Yields of Ash Rate coal Coal activated (ZnCl % 10 % Coal activated (NaOH % 12% Coal activated ( H % 9% Physico-cheical characterization of the odified bentonite Maghnia The bentonite used in our work is extracted fro Haa-Boughrara at Maghnia (Tlecen. Our finely ground was provided by the copany ENOF bentonite of Maghnia (Tlecen, Algeria. Bentonite is a ixture of ontorillonite, kaolin, and quartz and calcite ipurities. The specific surface area is /g. The ph is The Table 4 and Table 5 showed the results of analysis of the cheical coposition of the clay used. ENOF (National business nonferrous ining products. Density related (kg -3 Table 4. Bentonite cheical coposition of Maghnia (Algeria Constituents SiO 2 Al 2O 3 CaO MgO K 2O Na 2O Percentage (% Table 5. Physical properties of the ontorillonite Maghnia (Algeria true density ph Specific pore volue Fire loss Huidity (kg -3 surface (l g -1 (% ass (% ( 2 g -1 Color White Results and Discussion Spectrophotoeter UV-visible, benzoic acid deterination ethods Analyses are perfored on a Shiadzu spectrophotoeter 8543 odel controlled by a coputer. The highest wavelengths are obtained by autoatic scanning between 200 and 800 n. Quartz cell of (1 c optical path are used. Witness s solutions without adsorbents are prepared to ensure that there is no interference with tie (Bouras, 2003.The benzoic acid assay is carried out in the UV with a wavelength of 271 n corresponding to the axiu absorbance. 40

4 Aceh Int. J. Sci. Technol., 5(1 : ax Table 6. Maxiu wavelength of benzoic acid DO ,039 0,036 0,051 0,047 0,097 0,142 0,177 0,23 0,219 0, ax DO 0, (a (b DO y = x R² = C (g/l Figure 1. UV-visible spectru of benzoic acid, Wavelength benzoic acid. (a Wavelength benzoic acid, ((b Curve benzoic acid calibration DO= C e Modeling the adsorption isother (Kinetics and Therodynaics on the adsorption of benzoic acid of the activated coal and bentonite Modeling of the equilibriu data was done using Freundlich and Languir isothers. The Languir equation is the ost widely used two-paraeter equation, coonly expressed (Nakagawa, 2004 c eq q (1 Ceq 1 k l q q x / q. q k C Where: Ceq = equilibriu concentration of adsorbate in solution after adsorption; x/ = aount adsorbed per adsorbent unit weight; and k l and q are the Languir constants. Fro a plot of Ceq/(x/ versus Ceq, k l (g/g and q (L/g can be deterined fro the slope and intercept, respectively. At equilibriu conditions, the adsorbed aount x/ can also be predicted using the Freundlich equation x 1. / n k F C eq (3 log x logk l eq 1 log n F C eq Where k f is an indication of the adsorbent capacity and 1/n is a easure of the surface heterogeneity, ranging between 0 and 1, becoing ore heterogeneous as its value gets closer to zero. Using Eq. (3 fro the plot of log x/ versus log C eq, the paraeters n and k were obtained fro the slope and intercept, respectively. Since the analysis of the isother is iportant in order to develop an equation that accurately represents the results and which could be used for design purposes, two have been applied in this study, the Languir (1, Freundlich (2 out of the several isother equations. Adsorption odel constants, the values which express the surface properties and affinity of the adsorbent, can be used for our Coal saple. The paraeters in the odels were estiated by nonlinear regression and by fitting transfored data to the linear fors of the odels. A total of 500 l aqueous solution of benzoic acid definite initial concentration Ci equal to 70g/l are contacted with a ass of 1g of crude coal, activated (NaOH, ZnCl 2, H 3 and Bentonite, under agnetic stirring at roo teperature and ph = 4 for different contact ties. When the equilibriu state of the solution thus prepared is reached, the solution undergoes a centrifugation 1500tr /in. (4 (2 41

5 Aceh Int. J. Sci. Technol., 5(1 : Influence of the ass of the (Coal and bentonite on the adsorption of benzoic acid The study is perfored as above for the benzoic acid solution, for each ass (coal and bentonite 0.2, 0.3, 0.4, 0.5, 0.8, 1g, the initial concentration of solution Ci = 70g /l The ass of the activated coal (NaOH, ZnCl 2, and H 3 and optiu bentonite for benzoic acid is fro ( g the shape of the curves 03 having a vertical slope and linearity arked until the state of equilibriu. Isother of binding of benzoic acid on activated coal and bentonite 1g (coal activated by ZnCl 2, NaOH, H 3 and bentonite each added aterial 100 l of an aqueous solution of benzoic acid concentration definite the experient is repeated with other benzoic acid concentration, 15, 20, 30, 40, 50, 60 and 70g / l to only studies the influence of the concentration on the adsorption, the ph is kept constant at its optiu value (4, and the solution is stirred continuously. The Ceq concentration is easured by UV spectrophotoeter. Have been found that raw coal efficiency is not as iportant as the activated coal by (H 3, NaOH, ZnCl 2 and bentonite; because its efficiency of retention of benzoic acid at equilibriu is 2.81% after 70 in which is a value lower than that of activated coal (H 3, NaOH, ZnCl 2 and bentonite as retention yields of 40.98, 18.82, 17.3 and 49.3% respectively. Both coal treated with ZnCl 2 and NaOH have adsorption speeds 1,774 g / l.n and 2.014g / l.n successively; rearkable speed is raised to the saple of coal treated with ortho-phosphoric acid 3.98g / l.n. Benzoic acid has a better adsorption on coal treated with ortho-phosphoric acid, having a icro pore surface area greater than that of the odified bentonite, so increasing the porosity of the vase increases activated retention the benzoic acidthe axiu aounts absorbed by these three saples of the coal activated H 3, NaOH and ZnCl 2 are of the order of 14.34g / g 6.16 g / g and 6.58 g / g respectively. This bentonite adsorption rate of 2.7 g / l.n and the axiu quantity fixed 6.9 g / g. Thus, the clay, which has a high surface area, better adsorbed benzoic acid. Raw coal for the adsorption speed is 0.05g / l.n and the axiu quantity specified 0.98g /g, we represent in the Figures 2c and Figure 2d. The adsorption isothers of benzoic acid on the adsorbent of the raw coal, activated (ZnCl 2, NaOH, H 3 and Bentonite linearity s fro the relationship Freundlich. Absorption capacities of benzoic acid on these saples of the coal and the bentonite can be classified as follows: n Bentonite > n Coal ( H 3 > n Coal ( ZnCL 2 > n Coal ( NaOH > n raw Coal. The residual coal treated with phosphoric acid gives the best results aong the studied adsorbents studied. The figure 2d represent the Languir adsorption isother according to the relationship x / q. q k C l eq there as the value 99% obtained for the factor that characterizes the linearity of the plot is estiated sufficiently acceptable to say that this isother obeys to odel. Table 7. Freundlich isother paraeters for l'adsorption benzoic acid using coal (raw and enabled and bentonite n <1: low adsorbent n> 1: good adsorbent Freundlich equation: log x logk 1 log n F C eq n Kf R 2 activated coal with ZnCl low adsorbent activated coal with H good adsorbent activated coal NaOH 1.99 good adsorbent the raw coal 0.48 low adsorbent Bentonite 3.5 good adsorbent

6 Aceh Int. J. Sci. Technol., 5(1 : coal activated by (H 3 coal activated by (NaOH coal actvated by (ZnCl 2 crude coal (Bentonite coal activated byzncl 2 coal activated by (NaOH coal 1,6 activated by(h 3 crude 1,4 coal Bentonite 1,2 1,0 0,8 C ads 15 0, Teps n Log x/ 0,4 0,2 0,0-0,2-0,4 0,4 0,6 0,8 1,0 1,2 1,4 1,6 1,8 Log C eq x/ (g/g (a coal activated by(naoh coal activated by (ZnCl 2 coal activated by(h 3 Bentonite 1/x/ 1,8 1,6 1,4 1,2 1,0 0,8 0,6 (b coal activated by (ZnC l2 coal activated by(naoh coal activated by(h 3 crude coal Bentonite 1 0,4 0 0,2-1 0,0 0,2 0,4 0,6 0,8 1,0 (g 0,0 0,00 0,05 0,10 0,15 0,20 0,25 0,30 0,35 0,40 x/ (c Figure 2. Freundlich and languir adsorption isother for benzoic acid by crude, activated Coals and Bentonite, (a Effect of contact tie on the reoval of benzoic acid (Coal crude, activated and Bentonite, (b Freundlich adsorption isother for benzoic acid by crude, activated Coals and Bentonite, (c Influence of the ass (the activated coal and the odified bentonite on the reoval of benzoic acid, (d Languir adsorption isother for benzoic acid by activated, raw coal and Bentonite Conclusions This work show the interest of the local clay and coal (fro Algeria in environental technology for the treatent of Coposed Organic (benzoic acid which originates fro an industrial pollution (petrocheical plants, refineries, paper ills.the abundance of clay aterial is not the only advantage, but it's really a cost-effective natural adsorbent for organic copounds. The abundance of clay aterial is not the only advantage, but it's really a cost-effective natural adsorbent for organic copounds. The adsorption of benzoic acid was studied by following the ethod of spectrophotoetric assay ethod. Adsorption tests of benzoic acid indicate that bentonite and coal can be used as adsorbent of organic copounds given its abundance and low cost. For the sae concentration and for the sae flow rate, the tie to breakthrough and saturation increases with increasing retention. Models of Languir, and FREUNDLICH were applied to the experiental data obtained fro therodynaic studies of fixed bed to provide the breakthrough curves. All odels are generally well siulated to describe all or part breakthroughs curves of benzoic acid on clay and natural coal Algeria. References Akçay, M. and Akçay, G The reoval of phenolic copounds fro aqueous solutions by organophilic bentonite. Journal of Hazardous Materials, 113(1-3: Bared, R., Boucheta, A., Chaib, M. and Kacii, S Phenol and benzoic acid degradation by Pseudoonas aeruginosa. Journal of Water Resource and Protection, 2: (d

7 Aceh Int. J. Sci. Technol., 5(1 : Boucheta, A., Bared, A., Chaib, M., Kacii, M. and Kadouri, N Phenol adsorption fro crude and active coals. Journal of Water Resource and Protection, 2: Bouras, O Propriétés adsorbantes d argiles pontées organophiles synthèse et caractérisation. These Pour l obtention du grade de Docteur de l université de lioges. Deul, M. and Annell, C.S Occurrence of inor eleents in ash of low-rank coal fro Texas, Colorado, North Dakota, and South Dakota. U.S. G.P.O Books, California. Eren, E. and Afsin, B Reoval of basic dye using raw and acid activated bentonite saples. Journal of Hazardous Materials, 166(2-3: Graiyna, G Effectiveness of high teperature pyrolysis in sulphur reoval fro coal. Elsevier, New York. Loison, R., Foch, P. and Boyer, A Coke quality and production. Ed Butter Worths, e-book. ISBN CERCHAR (Centre d'etudes et Recherches de Charbonnages de France X: Nakagawa, K. Naba, A., Mukai,.S.R. and Taon, W Adsorption of phenol and reactive dye fro aqueous solution on activated carbons derived fro solid wastes. Water Research, 38(7:

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