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Fluoridated groundwater treatment using natural and calcined magnesite and gypsum: System optimization based on laboratory studies on adsorption kinetics and thermodynamic considerations
KTH, School of Architecture and the Built Environment (ABE), Sustainable development, Environmental science and Engineering, Water and Environmental Engineering. Department of Water Resources Engineering, University of Dar es Salaam, Dar es Salaam, Tanzania;Department of Chemistry, University of Dodoma, Dodoma, Tanzania. (KTH-International Groundwater Arsenic Research Group)ORCID iD: 0000-0003-3270-5438
KTH, School of Architecture and the Built Environment (ABE), Sustainable development, Environmental science and Engineering, Water and Environmental Engineering. Department of Water Resources Engineering, University of Dar es Salaam, Dar es Salaam, Tanzania;Department of Transportation and Geotechnical Engineering, College of Engineering and Technology, University of Dar Es Salaam, Dar Es Salaam, Tanzania.ORCID iD: 0000-0002-7435-1677
KTH, School of Architecture and the Built Environment (ABE), Sustainable development, Environmental science and Engineering. Department of Water Resources Engineering, University of Dar es Salaam, Dar es Salaam, Tanzania.ORCID iD: 0000-0002-2883-2445
KWR Water Research, Nieuwegein, The Netherlands.
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Fluoride (F-) is one of the key water quality parameters of concern due to its impact on human health. High F- intake has resulted in the development of dental and skeletal fluorosis in several countries, and removal of F- from drinking water sources is important for securing the drinking water sources. The batch experiment was performed to determine the optimum parameters for F- removal using calcined gypsum and magnesite. The optimum heating temperature, dosage, and contact time were found to be 350 °C, 100 g/L, and 40 min, respectively, for gypsum, and 650 °C, 20 g/L, and 36 min, respectively, for magnesite. The adsorption process on the surface of calcined gypsum and magnesite was well explained with the pseudo-second-order kinetic. The experimental data fitted well to the Freundlich isotherm model in both adsorbents with   values of 0.0303 mg/g for gypsum and 1.3505 mg/g for magnesite. The values of Gibbs free energy ( ΔGo) and enthalpy ( ΔHo) indicated that the F- adsorption on the gypsum surface was spontaneous and exothermic, while that on the magnesite surface was spontaneous and endothermic. The concentration of F- in water treated by gypsum was 1.99 mg/L, slightly above the World Health Organization (WHO) but within Tanzania Bureau of Standards (TBS) guidelines. Water treated by magnesite has F- concentration below WHO standards and a pH above the WHO and TBS guidelines, so the pH needs to be adjusted before water can be used for drinking.

Keywords [en]
Batch experiments; Calcined magnesite, Calcined gypsum, Adsorption process, Mineral phases, Adsorption isotherms
National Category
Environmental Engineering
Research subject
Land and Water Resources Engineering
Identifiers
URN: urn:nbn:se:kth:diva-327346OAI: oai:DiVA.org:kth-327346DiVA, id: diva2:1759064
Funder
Sida - Swedish International Development Cooperation Agency, 51170071
Note

QC 20230525

Available from: 2023-05-24 Created: 2023-05-24 Last updated: 2023-05-25Bibliographically approved
In thesis
1. Groundwater defluoridation by natural minerals: Understanding the process of fluoride removal from drinking water sources in Tanzania
Open this publication in new window or tab >>Groundwater defluoridation by natural minerals: Understanding the process of fluoride removal from drinking water sources in Tanzania
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Fluoride (F-) concentration in drinking water is one of the water quality parameters in countries with high concentrations in groundwater sources. Natural minerals have shown considerable effectiveness in F- removal. In this study, the performance of the locally available natural minerals, such as bauxite, magnesites, and gypsum, have been investigated at the laboratory scales and through modelling for F- removal from drinking groundwater sources in Tanzania. Batch experiments were carried out to examine the optimum conditions for F- removal by the calcined bauxite, magnesite, and gypsum. X-ray fluorescence spectroscopy (XRF) characterization showed that Al2O3, MgO, and SO3 were the major oxides in bauxite, magnesite, and gypsum, respectively. The experimental data for the three treated adsorbents fitted well with the Freundlich adsorption isotherm and the pseudo-second-order kinetics. The values of ∆G° and ∆H° indicate that the F- adsorption on bauxite and magnesite surfaces was spontaneous and endothermic. The randomness described by ∆S° at the solid–liquid interface was increased during the adsorption processes. While for gypsum, the reaction was spontaneous and exothermic, where the randomness at the solid–liquid interface decreased during the adsorption processes. At optimum conditions, calcined bauxite (400 °C), magnesite (650 °C), and gypsum (350 °C) lowered the F- concentration from 8.27 mg/L to 1.02, 0.233 and 1.99 mg/L, respectively. Bauxite and gypsum lowered the pH of water from 9.38 to 6.74 and 7.41, respectively. Magnesite raised the pH from 9.38 to 10.12, which is above the World Health Organization (WHO) (6.5 - 8.5) and Tanzania Bureau of Standards (TBS) (6.5 – 9.2) drinking water standard; therefore, pH adjustments are needed before water can be used for drinking. The Bed Depth Service Time (BDST) plot showed that the service times for F- adsorption on the calcined bauxite and magnesite surface increased with bed depth. The critical bed depths (Zo) for bauxite and magnesite obtained were 7.21 and 8.28 cm, respectively. The lower value of the kinetic rate parameter (Kα) for bauxite (1.43E-5 L/mg s) and magnesite (1.50E-5 L/mg s) highlighted that the breakthrough occurs in short beds; therefore, deeper beds are required to avoid breakthroughs. The experimental results and model predictions have helped to compare the adsorption processes as well as contrast their performance and sustainability for F- removal using the bauxite, magnesite, and gypsum in the drinking water resources in Tanzania. The adsorption results and the overall cost analysis show that the cost of calcined bauxite and magnesite is low compared to other available adsorbents; therefore, they can be used in F- removal from water.

Abstract [sv]

Förhöjda koncentrationer av fluorid (F-) i grundvattnet är en av vattenkvalitetsparametrarna som utgör en betydande utmaning för säker dricksvattenförsörjning i flera länder globalt. Naturliga mineraler har visat avsevärd effektivitet för att avlägsna fluor. I denna studie har prestandan hos de lokalt tillgängliga naturliga mineralerna, såsom bauxit, magnesit och gips, undersökts i laboratorieskala genom modellering av fluoridavlägsnande från grundvattenkällor i Tanzania. Batchförsök utfördes för att undersöka de optimala förhållandena för F- borttagning av den kalcinerade bauxiten, magnesiten och gipsen. Röntgenfluorescens (XRF) spektroskopisk karakterisering visade att Al2O3, MgO och SO3 var de viktigaste oxiderna i bauxit, magnesit respektive gips. Experimentell data för de tre behandlade adsorbenterna följde väl med Freundlich-adsorptionsisotermen och pseudo-andra ordningens kinetik. Värdena för ∆Go och ∆Ho indikerar att F- adsorptionen på bauxit- och magnesitytor var spontan och endoterm. Slumpmässigheten, som beskrivs av ∆So vid gränsytan mellan fasta fasen och vätskan, ökade under adsorptionsprocesserna. Medan för gips var reaktionen spontan och exoterm, där slumpmässigheten vid gränsytan mellan fasta fasen och vätskan minskade under adsorptionsprocesserna. Vid optimala förhållanden, sänkte kalcinerad bauxit (400 °C), magnesit (650 °C) och gips (350 °C) F- koncentrationen från 8,27 mg/L till 1,02, 0,233 respektive 1,99 mg/L. Bauxit och gips sänkte vattnets pH från 9,38 till 6,74 respektive 7,41. Magnesit höjde pH-värdet från 9,38 till 10,12 vilket är över pH-intervallet mellan 6,5 - 8,5 och 6,5 - 9,2 som rekommenderats av Världshälsoorganisationens (WHO) riktlinjer för dricksvatten och Tanzania Bureau of Standards (TBS). Därför justering av pH behövs innan det behandlade vattnet kan användas för dricks ändamål. Designmodellen för bädd djupsservicetid (BDST) användes för att karakterisera genombrottsprocesserna. De kritiska bädddjupen (Zo) för erhållna bauxit och magnesit var 7,21 respektive 8,28 cm. Bädddjupsservicetid (BDST)-plotten visade att servicetiderna för F- adsorption på den kalcinerade bauxit- och magnesitytan ökade med bädddjupet. Det lägre värdet på kinetisk hastighetsparameter (Kα) för bauxit (1,43E-5 L/mg s) och magnesit (1,50E-5 L/mg s) visade att genombrottet sker i korta bäddar; därför krävs djupare bäddar för att undvika genombrott. De experimentella resultaten och prediktionsmodellena har hjälpt till att jämföra adsorptionsprocesserna samt kontrastera deras prestanda och hållbarhet för avlägsnande av fluor med hjälp av bauxit, magnesit och gips i dricksvattenresurserna i Tanzania. Adsorptionsresultaten och den övergripande kostnadsanalysen visar att kostnaden för kalcinerad bauxit och magnesit är låg jämfört med andra tillgängliga adsorbenter; därför kan de användas vid F- borttagning från grundvatten.

Abstract [sw]

Mkusanyiko wa floridi (F-) katika maji ya kunywa ni mojawapo ya vigezo vya ubora wa maji katika nchi zilizo na ukolezi mkubwa wa F- katika vyanzo vya maji. Madini ya asili yameonyesha ufanisi mkubwa kwa kuondolewa kwa F-. Katika utafiti huu, utendaji wa madini asilia yanayopatikana humu nchini kama vile bauxite, magnesite na jasi umechunguzwa katika mizani ya maabara na kutoa mfano wa kuondolewa kwa F- kutoka vyanzo vya maji ya chini ya ardhi nchini Tanzania. Majaribio ya kundi yalifanywa ili kuchunguza hali bora za uondoaji wa F- kwa bauxite iliyokatwa, magnesite na jasi. Tabia ya uchunguzi wa uchunguzi wa X-ray fluorescence (XRF) ilionyesha kuwa Al2O3, MgO na SO3 zilikuwa oksidi kuu katika bauxite, magnesite na jasi, kwa mtiririko huo. Data ya majaribio ya adsorbenti tatu zilizotibiwa ililingana vyema na isotherm ya Freundlich ya adsorption na kinetiki ya mpangilio wa pili wa uwongo. Thamani za ∆Gº, ∆Hº zinaonyesha utepetevu wa F- kwenye uso wa bauxite na magnesite ulikuwa wa pekee na wa mwisho wa joto. Nasibu iliyoelezewa na ∆Sº kwenye kiolesura kigumu-kioevu iliongezwa wakati wa michakato ya utangazaji. Ilhali kwa jasi majibu yalikuwa ya hiari na ya kupita kiasi ambapo unasihi kwenye kiolesura kigumu-kioevu ulipungua wakati wa michakato ya utangazaji. Katika hali bora zaidi, bauxite iliyokaushwa (400 °C), magnesite (650 °C), na jasi (350 °C) ilipunguza mkusanyiko wa F- kutoka 8.27 mg/L hadi 1.02, 0.233 na 1.99 mg/L, kwa mtiririko huo. Bauxite na jasi zilipunguza pH ya maji kutoka 9.38 hadi 6.74 na 7.41, kwa mtiririko huo. Magnesite ilipandisha pH kutoka 9.38 hadi 10.12 ambayo ni juu ya Shirika la Afya Duniani (WHO) (6.5 - 8.5) na Shirika la Viwango Tanzania (TBS) (6.5 – 9.2) kiwango cha maji ya kunywa, kwa hiyo marekebisho ya pH yanahitajika kabla ya maji kuongezwa. kutumika kwa kunywa. Mpango wa Muda wa Huduma ya Kina cha Kitanda (BDST) ulionyesha kuwa nyakati za huduma za F- adsorption kwenye uso wa bauxite iliyokaushwa na magnesite ziliongezeka kwa kina cha vitanda. Kina muhimu cha kitanda   kwa bauxite na magnesite zilizopatikana zilikuwa 7.21 na 8.28 cm, kwa mtiririko huo. Thamani ya chini ya kiwango cha mmenyuko mara kwa mara (Kα) kwa bauxite (1.43E-5 L/mg s) na magnesite (1.50E-5 L/mg s) iliyoangazia mafanikio yatatokea katika vitanda vifupi; kwa hiyo, vitanda vya kina vinahitajika ili kuepuka mafanikio. Matokeo ya majaribio na utabiri wa modeli umesaidia kulinganisha michakato ya utangazaji pamoja na utofauti wa utendaji na uendelevu wa kuondolewa kwa F- kwa kutumia bauxite, magnesite na jasi katika rasilimali za maji ya kunywa nchini Tanzania. Bauxite iliyokaushwa na magnesite iliboresha uondoaji wa F-.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2023. p. 35
Series
TRITA-ABE-DLT ; 2332
Keywords
Fluoride removal, Groundwater, Natural minerals, Adsorption isotherms, Batch- and Column Experiments, Kinetics and thermodynamics, Drinking water quality, Sustainability, Kuondolewa kwa fluoride, Maji ya chini ya ardhi, Madini ya asili, isotherms za majaribio ya adsorbenti, Majaribio ya Kundi- na Safu, Kinetics na thermodynamics, ubora wa maji ya kunywa, Uendelevu, Fluoridavlägsnande, Grundvatten, Naturliga mineraler, Batch- och kolonnförsök, Adsorptionsisotermer, Kinetik och termodynamik, Dricksvattenkvalitet, Hållbarhet
National Category
Environmental Engineering
Research subject
Land and Water Resources Engineering
Identifiers
urn:nbn:se:kth:diva-327348 (URN)978-91-8040-623-9 (ISBN)
Public defence
2023-06-14, Two venues: Sahara, Teknikringen 10B, KTH Campus, Sweden at 13:00 (CEST), AND Swedish Embassy at Dar es Salaam, Tanzania at 14:00 (EAT), video conference link: https://kth-se.zoom.us/j/64600615013, Stockholm, 13:00 (English)
Opponent
Supervisors
Funder
Sida - Swedish International Development Cooperation Agency, 51170071
Note

QC 20230525

Available from: 2023-05-25 Created: 2023-05-24 Last updated: 2023-06-27Bibliographically approved

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Kimambo, VivianIjumulana, J.Ligate, Fanuel JosephatBhattacharya, Prosun

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