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.) Journal of Chemical Engineering & Proce: = s Technology Scrubbing of HCI Gas from Synthesis Gas in a Multistage Dual-Flow Sieve Plate Wet Scrubber by Alkaline Solution ‘Swamy Kurella!, Mounika Balla’, Pavan Kishan Bhukya! and Meikap BC" "Deparment of Crome! Enginsering, nslon neta of Tecnology Khargpur naa “Depertnen of Chemeal Engnetng, Scho! of Chemical Enginoaring, Howard Calege Campus, Unversty of Kwezu-Naal(UKZN), Durban, South Atice Abstract, hydrogen slp and nyaragen close ‘fom eftuort gas sbaam.Dual'fow sive pate colann wet scuBbars can Bows {o remove ts HCI fom te syntnoss gas a ores gabqu ratos wine to gas ow rats (2) 8.297» 10" Nr, 13.829» 10" Nie and 19.38% 10" Nah Now rates (,) 20868" Tose 94415 «1oemts and 48:18 > TO" and at ren kt Hl concanvatons (Cy)100 ppm, 200 pom and 300 pom range using scdum njcrxte saluton as seruDsing qu The mam pecertage removal of Hl (in. 84.8% are observed ok Qy-8 297 = 10° Nii, Q,~ 48-189» 10" ie and Cy=800 pp wih Eons knot’ NaOH soliton. Adem enprel model hasbeen devloped fo pred! he efcency ofthe HCl sebbing eng the "xpormental ests an the varbles when show the impact onthe suber prlomanee. Almost AO" the experimental reals fre matches wollwih te predict vaios wih oss an 5% dovatn, Keywords: Air polluion: Control, Elicency: Scrubbing: Mode; Removal: Sodium hydroxide Introduction Coal i a combustible substance composed of carbon along several impurities like sulphur, chlorine, and nitrogen and metal ‘compounds. These impurities get converted to gaseous species such as 11S, HCL and NH, when this coal is processed. Therefore, removal ‘of these impurities is essential to protect the energy production ‘equipment and to meet environmental standards before entering into the atmosphere. During the gasification process, the chlorine pres in the coals volatiized to HCl or metal chlorides. The chloride conten i high in US coals with 01019 to 0.9% and during coal gasifieation process these chlorides will produce HCl [1], In the gasfiation proces, the chlorine content of coal volatiizes to metal chlorides or HCL, But major portion of chlorine is converted into HCL Reporte shovr that there is a wide variation in the LC] concentrations in synthesis gas streams. Bakker and Perkins [2] reported that the HCL ‘concentration ie five times higher in coal gas than in coal-fired boiler ‘combustion gat stream. The chlorine content of coal, the gasification temperature and the type of gasifier are the factors on whieh the HCL vapour concentration depends and the most reliable data was found from the fixed-bed gasifier aperation at General Electric Corporate Research and Development at Schenectady, New York At that facility about 300 ppm FCI vapour concentration was obtained using coal ‘with 0.24 wis chlorides [3]. The concentrations of HCl are reported as high az 500 ppm in coal syngas from gasifier eluents [4,5]. Pekins et al. [6] reported thatthe chloride deposited on syngas coolers accelerate the corrosion of the heat exchanger material and HCI reacts with the deposited scum of sag, forming low-melting iron chlorides, thereby ‘expediting the corrosion rate, ICI gas destroys the metal and lime stone building structures due to its highly corrosive nature. HCl is harmful to aquatic organisms ‘when it is highly dissolved in water and many times it ile them. The ‘emitted HCI into the environment is quickly washed out by moisture inthe ai and rain, Ifthe HC levels in these acid rains are above the ‘exposure limits then the lakee and sols will be affected [7]. Exposure to high concentrations of HC! emissions leads to various health issues such at skin colour change, rapid breathing and fluid accumulation in the lungs. HCI gas ingestion seriouly destroys the gust and in exteme cases teases to death also Frank and Nancy [8] ave reported that the wet scrubbers are fective air polltion control devices which can simaltancously remove both gaseous pollutants and dust particles. Wet scrubber removes partclesby capturing them in liquid droplets, and they remove garesby Aisrolving or absorbing them into the liquid [3]. The gaseous pollutants ‘will be removed in the wet scrubbers by absorbing or dissolving them into the serubbing liquid and for FIC ges removal this srubbing quid isnormally water ora weak alkaline solution, In many cases, weak basic solutions give higher HCI gas removal eficiencies than ordinary water, Furthermore, the efciencies of dry scrubbing methods are relatively low compared with wet scrubbing methods ‘There are diferent types of serubbers reported in the literature to choose the suitable serubber for particulate and gaseous pollutant removal with higher removal efficiencies [10-14]. Rsjmoban etal. [10] Ihave reported almost 99.99% SO, removal eficiency of twin uid ai. assist atomized spray column, Meikap et al. (11] have reported the water scrubbing and alkali (NsOH) serubbing of SO, gas using small droplets in horizontal co-current flow ejector system with $8,625 and 100% removal eficiencies respectively. ‘The SO, gas scrubbing thas also been studied with greaer removal efficiencies in a modified multistage bubble column serubber without using any additives or pre-treatment [12]. Bandopadhyay et al. [13] have achieved almost 00% removal eficiencies with akal rubbing of SO, ga in a Tapered School of Campi, University of KaZueNail (URN), Dur Email: omokap@tehe.ekgpomotn Detooer as, 2018 Citation Krall S, Gla M, Bhkya PK, Moka BC (2015) Seubbing of HI Gas ‘fom Syrtnss Gas na Nustage Dut Fow Seve Pst Wel Seubbe’b/ Copyright: © 2015 Kiel, at Tis an open-access atl etbutd under ‘ho terns of he Cente Commons Atrbuton Lcons, whch permits Unesses 1S, dsubuton and producton in any meaum. provides a og auha a Citation: Kurela S, Bala M, Bhukya PK, Meikap BC (2015) Scrubbing of HCI Gas for Synthesis Gas in a Mulistage Dual-Flow Siove Plate Wel Scrubber by Alkaline Solution, J Chem Eng Process Techndl 6: 250, dl 10.4°7212 57-7048, "000250 Bubble Column Scrubber. Bangyroo Han etl, (14] have observed the THEI removal in a packed bed scrubber for four different packing at various liquid-gae ratios. There is very les Ierature found for gae absorption in multistage dual-iow sieve plate columns. The mest ‘commonly used perforated tray column without a down comer is one ‘of the dual-flow tray column, whichis used for its simple design and its eae of installation and maintenance, In many applications the dual flow trays were used where there is no need of wide range of operating ‘conditions, Inthe operating range, with the less capital investment it fiver high maze transfer efficiency. The alternating counter passage of gas and liquid through the holes provides a self-cleaning fof the device in fouling systems [15.16]. This paper presents the work done for the removal of HCl gas from an effluent gse stream with a three stage dual-low seve plate column wet scrubber and the effect ‘of different operating variables on HC removal efficiency of scrubber, ‘Materials and Methods Materials Hydrochloric acid solution (35%), sodium hydroxide pellets of 97% ac Air Compressor He HCI Container Ik Impingers MytoMs Pressure Ports P Pomp Rik Rotamctes s Shumry Tank SiSt Sample Ports T Water Teak VitoVi Valves Vw Veanusi Mixer purty, oxalic acid dehydrate of 99% purity were supplied by Merck Specialities Pvt, Ltd. and used without further purification. Aqueous solution of hydrochloric aid, dilute oxalic aid solution (0.025 k moti ‘m’) and dilute galation# of sodium hydroxide (0.00125 k mol/m,0.0025 kc mol/m’ 0.00375 k mol/m, 0.005 k mol/m and 0.05 k mol/m’) have ‘been prepared using distilled water. Dilute Hydrochloric acid solution was prepared by dissolving 35% pure concentrated hydrochloric acid in distiled water (0.6 kmol/m'- 2k moll) Methods “The schematic representation ofthe experimental set-up is shown in Figure 1. A three stage dusl-flow sieve plate column is made up of a tansparent, vertical Perspex glass with 2.6 m length and 0.1524 sm ID and fitted with an outet at top in fructo-conical shape. ‘The air contaminated with HCL enters through the inlet ofthe column, Theinlet is ited with a dlfurer on the inner side ofthe column to facilitate the flow of the gasina uniform manner throughout the column The plates and diguser consist of 396 holes of 3 10” m size. The experimental air for the operation is supplied by an air comprestor which was prepared. by sucking the ambient air The outlet ofthe air compressor is fited Fv Ree Q Figure: Schomate agra of xporimortal up. Citation: Kurela S, Bala M, Bhukya PK, Meikap BC (2015) Scrubbing of HCI Gas for Synthesis Gas in a Mulistage Dual-Flow Siove Plate Wel Scrubber by Alkaline Solution, J Chem Eng Process Techndl 6: 250, dl 10.4°7212 57-7048, "000250 to an air rotameter of range 0-27.65 x 10 Nm’, The outlet of the rotameter is connected to the inlet of the column t mixer, Liquid HCl of known concentration is placed ina ‘bottom flask of one litte capacity Part of the experimental air was ‘entered into the flask from one end and bubbled into the concentrated liquid HCI to form the HCl vapours. The generated HCI vapoure were then allowed to excape through the other end to enter into the ventari _mixer where they were mixed with the other part ofthe experimental ait and enter to the column at desired concentrations, The concentrations ‘of HCl are maintained at desired valuee with less than + 5% deviations ‘A tank of 20 x 10° m’ capacity is used ae liquid reservoir from which the scrubbing liquid is pemped out by 20.5 HP centrifugal pump to the column at the top where a lguid distributor plate disperses the liquid to the try below in a chower manner. ‘Ihe flow rate ofthe scrubbing liquid ie controlled through arotameter of range 0-68.83 « 10° ms, “Theexperimental conditions canbe seen in Table, The experiments were conducted at different gas to ligsid ratios at diferent inlet HCL concentrations, The samples were collected at S, and S, which are sample porte at inlet and oudet respectively. For iso-kinetic sampling {60 x 10 m'of 005 k mol/m' NaOH solutions was placed in the three impingers in series in which the first impinger inlet was connected to the sample port and the third impinger outlet was connected to ‘vacuum pump and gas meter. As the experiment proceeded, the HCL ‘vapours were passed through the impingers and got absorbed into the [NAOH solution. The NaOH reacts withthe HCL in the contaminated air, thereby, neutralizing it, Treated sir is then discharged into the atmosphere. Ae the reaction proceeds, the concentrations of NaOH solution in the impingers get reduced and they were estimated by titrating agsinst Oxalic Acid. The amount ofHICL abeorhed is evaluated by back calculation and the concentrations of HCL at islet (Cys aye and outlet (Cp gg) Were calculated, The percentage removal of HCL (én) of the column i calculated from the equation (1). ‘mollim’ and 0.005 k mol/m are sed as serubbing liquids. HCI zemoval ciency percentage has been estimated using equation (1). Effect of liquid flow rate and HCl loading on the percentage removal of HCL ‘The scrubbing liquid flow rate effect on HCl percentage removal bas been shown in Figures 2-4, for 0.005 kmalimy? NaOH solution and for diferent constant gas low ratesat 100 ppm, 200 ppm and 300 ppm inlet, HCI concentrations respectively, Its abserved from the results thatthe Hl percentage removal increased withthe increate in higuid flow rat, ‘Aste liquid low rae increases the avalablity of mass transfer surface ncreates which increases the interfacial contact between the liquid and gas [17] andthe high eactive nature of NAOH reacte with HCI vapours as soon as they are absorbed into the liquid phase NaOH (scrubbing iquid). Due to this fact, the HCI removal efficiency of the dua-flaw sieve plate scrubber increases with increasing the flow rate of liquid “The mechanism involves in the dual-flow sieve plate column is that the liquid and gar flows through the holes in counter curre alternatively. There are two zones in each stage namely ftath and spray. In the froth zone, the up flowing gas passes through the thin iguid layer in small bubbles form and in the spray zone the down flowing guid from the above tray flows in streams and breake into droplets, ‘Many times the mass transfer occurs in both the zones significantly [15]. tis also observed thatthe efficiency increased with the increase in concentration due to the fat that the increased concentration increases the gradient of concentration between the gie phase and liquid phase HCI concentrations which directly improves the driving force for absorption of HCl into the film of serubbing liquid on the tray and the iquid droplets coming from the above tay Similar trends of results are ‘obtained and observed with the NaOH solutions of 0.00125 k mol/z’, (0.0025 k mol/m" and 0.00375 k mol/m? concentration. Effect of gas flow rate and HCI loading on the percentage Cyexaia — removal of HCL ye, = Pt 109 ® Cyc From the Figures 5-7 the effect of gas flow rate on HCl percentage Results and Discussion 0 “The experimental study was conducted to observe the removal of os Hin three stage dual fow seve plate column wet scrubber wth water and diferent concentrations of NaOH solutions as serubbing liquids. ” Effects of various parameters such as low rate of gas, flow rate of liquid Eas {inlet concentration of HCI and concentration of NaOi solution on e percentage removal of HCI are keenly observed, Experimentation has x” been done at various liquid rates of 20.649 x 10° ms, 44415 x 10° os n/sand 48,183 10 mls ad gas rates of 8297 10" Ns, 13.829 x = 10*Nav/s and 19.36% 10" Nm at dillerent inlet HCl concentrations 7” 100 ppm, 200 ppm and 300 ppm, Water snd diferent concentrations Bw ‘of NaOiH solutions af 0.00125 k mol/m’, 0.0025 k mol’, 0.00375 k Ey noe ie qu Fw ale (20.649 104,34 18 » 10% ad 48,183» 10" Ts 6 (cas tow rates 297x104, BED» 10" and 18.35 EN ‘souvbing ues [Te Wee ert Ne OH Solvers of erent ye ee ww 00, 20 and 300 pom “Table 4: Oparatng condone forthe Exgermantal Study of HCI removal in Mutisoge Dualilow Save Plate Colin, Liguid tow rate (Q, 10° ms) Figure 2: Eft of qu flow ato onto for HCl scrubbing with 0.005 kml PNGOH soluton a ferent constant gat rates and G00 pom. Citation: Kurela S, Bala M, Bhukya PK, Meikap BC (2015) Scrubbing of HCI Gas for Synthesis Gas in a Mulistage Dual-Flow Siove Plate Wel Scrubber by Alkaline Solution, J Chem Eng Process Techndl 6: 250, dl 10.4°7212 57-7048, "000250 | & 5 2 2 z g Liquid tow rate (Q, x10" ms) Figure 3: fest of qu ow rato on He flor HC setting wih 0.005 a [Srmbor x10" Na) e807 Liquid flow rate (Q, x10° mis) (pniedeneunle a ances Conan fw te ond a removal can be seen for 0.005 kmol/m’ NaOH solutions and for diferent constant liguid flow rates at 100 ppm, 200 and 300 ppm inlet HCI concentrations respectively. The results show that the increase in 42s flow rate decreased the HCI percentage removal. Tis is due tothe fact that the increase in gas flow rate decreases the residence time of gas phase in the column which further decreares the contact time between ‘the dow flowing liquid droplets and the up flowing gas in each stage andincreases the bubblerise velocity through the scrubbing iqui layer, ‘therefore the gas phase HCl absorption into the liquid phase decreases, which directly decreases the HCl percentage removal. The percentage removal of HClis mcressed withthe inlet ICI concentrations Effect of NaOH concentration on the percentage removal of HL 11 can be seen in the Figure 8 that the elect of NaOH solution {ymber @..0% wa] a mow Gas Now rate x10" Nas) Figure 5 Efectos fow ata onthe fr Hl sein 0.005 not on at ferent cans i ow ates an 6 °°00 po » » Symbat 10° ws g i i i é Gas flow rate (Q,x10° Nuv'is) Figure 6: Efecto ges fow ate onthe nfo HCl seutbing win 9.008 kml Citation: Kurela S, Bala M, Bhukya PK, Meikap BC (2015) Scrubbing of HCI Gas for Synthesis Gas in a Mulistage Dual-Flow Siove Plate Wel Scrubber by Alkaline Solution, J Chem Eng Process Techndl 6: 250, dl 10.4°7212 57-7048, "000250 = 0 Sos i EE Bs s° es Gas flow rate (Q, 10° N's) GON soon a feu cna Fed om es amc 300 pom concentration (C.,,) 0” percentage removal of HCI at different tnlet concentrations of HCI and at 8297 x 10" Nas ga flow rate, 48.183 « 10 mys liquid flow rate and it can also be observed that the HCl percentage removal eficiency increased with the increase in concentration of NaOH solution. It due to the fact that ae the concentration of NaOH increases the absorbed HCL into the higsid reacts as soon asitentersand directly enhances themasstransferintothe squid phase from the gas phase. Therefore asthe NaOH concentration increased the percentage removal of HCl in the multistage dual-flow sieve plate column serubber increased. Correlation development for removal efficiency prediction for water and NaOH scrubbing of HCl The liguid fow rate and gas flow rate effect on HCI percentage removal for 100 ppm, 200 ppm and 300 ppm constant inlet HCL concentrations at £297 x 10* Nae gue flow rate and 48.183 x 10° s/s liquid Dow rate can be seen in Figures 9 and 10 respectively. F the experimental data, Buckingham x theorem and choosing physical, geometsic and flow parameters an empirical equation bas been developed to predict the removal eflcency of HCL The parameters ‘which may influence the HCl removal efficiency (Njej-1,0 ) 2° (@) Geometrical parameters ~ scrubber height 11 (m), diameter of the column D,,(m) and sieve tray hole diameter d, (m), (b) Flow parameters - velocity ofgas V, (m/s) and velocity ofliquidV. (mis. te) Physical properties - 11Cl inlet concentration Ci kg/m’). density of Liquid p, (kg/m), density of gasp, kgm’), viscosity of gas, (kg/m), viscosity of liquid py (kg/ms),dilfusion coefficient of HCL in Water Dy (m/e) and gravitational acceleration g (m/s) The inlet concentration, ‘of LCLis exprested in kg/m’ for dimensional analyse purpose. Therefore, the removal eficiency of HCI becomes function of twelve parameters Ifthe relation existe theoretically between the HCL removal ficiency and the above system parameters then may be Mc writen inthe below form: £(d,,D.H,VosPorVisPLittosti»DsCyar8) Estimation of correlation coefficients of dimensional groups was done with multiple linear regression analysis. Neary the best Sted correlation with 0.1182 root-mean-square error (mse) and 0913 Coeficient of regression. The obtained model with the estimated coefcientsis given in equation (6) eecaiyialielay” Muc-m0 = zs ‘savrt0m zw aint’) Eo» Inlet HCI Concentration Cy, , PPM) Figure 8: Ect of Cys, 09 pocanage emeval of HC) sal, omer ‘Ste Cyc = 5 z $ zx Liquid Now rate (Q,310° 5) Figure 9: Ect of tld flow re on they fr water eeubbig st ‘foro contan Cys, 893 8.297» 10 Ni, Citation: Kurela S, Bala M, Bhukya PK, Meikap BC (2015) Scrubbing of HCI Gas for Synthesis Gas in a Mulistage Dual-Flow Siove Plate Wel Scrubber by Alkaline Solution, J Chem Eng Process Techndl 6: 250, dl 10.4°7212 57-7048, "000250 fa g0 be : i if» Gas flow rate (Q, x10" Nas) ‘fern constant and = a Tn equation (4), as the values of jes [2efand | 8) remained constant or their variation were negligible, olRecT [Rey] [Se] ° Peps P [se © Where k, and k are correlation constants and f is function of, variables Maa -m0 ug) “78710 [Re] ‘The major objective ofthis workis to analyze the HCl absorption in alkaline systess and prediction of the HCI remaval efficiency fr these systems. When HCI gas i absorbed into the water, reaction (A) occurs: HCL +109 11,, + Ch, a In particular situation of HCl absorption into aqueous NaOH solution, reaction (B) should be taken into account along with the reaction (A) Hi) FO, 22H,0 ® ‘With the overall eaction as HC1+NaOH > NaCl+H,0 © ‘The stoichiometric factor of reaction (C) i 1, therefore the mole ratio, x is ‘The interfacial concentration of HCL can be caleulated using ‘equation (7). The expression which has been used to estimate HCL cial concentration i, Crete =H ” H Where Gate interfical of HCL (kmol/m’), Hie the Henry's law constant (atm.m kml), Ps HCl partial pressure in bulk gas (atm). In the scrubber, the removal ficiency of HCL is depends on the tato of HCl mace transfer rates with and without chemical reaction. The HC percentage removal for allaline scrubbing (Mycr-wao)

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