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Implementation of Ion Exchange Processes on Industrial Waste Streams for Carbon Dioxide Mineralization- [electronic resource]
Implementation of Ion Exchange Processes on Industrial Waste Streams for Carbon Dioxide Mi...
Implementation of Ion Exchange Processes on Industrial Waste Streams for Carbon Dioxide Mineralization- [electronic resource]

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자료유형  
 학위논문파일 국외
최종처리일시  
20240214102125
ISBN  
9798380598378
DDC  
660
저자명  
Bustillos, Steven Juan.
서명/저자  
Implementation of Ion Exchange Processes on Industrial Waste Streams for Carbon Dioxide Mineralization - [electronic resource]
발행사항  
[S.l.]: : University of California, Los Angeles., 2023
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2023
형태사항  
1 online resource(142 p.)
주기사항  
Source: Dissertations Abstracts International, Volume: 85-04, Section: B.
주기사항  
Advisor: Simonetti, Dante A.
학위논문주기  
Thesis (Ph.D.)--University of California, Los Angeles, 2023.
사용제한주기  
This item must not be sold to any third party vendors.
초록/해제  
요약Sequestration of CO2 within stable mineral carbonates (e.g., CaCO3) represents an attractive emission reduction strategy as it offers a leakage-free alternative to geological storage of CO2 in an environmentally benign form. However, the pH of aqueous streams equilibrated with gaseous streams containing CO2 (pH 8). Traditionally, alkalinity is provided by a stoichiometric reagent (e.g., NaOH) which renders these processes environmentally hazardous and economically unfeasible. This work investigates the use of regenerable ion-exchange materials to induce alkalinity in CO2- saturated aqueous solutions such that the pH shift required for mineralization occurs without the need for stoichiometric reagents. Na+ -H+ exchange isotherms (at [H+ ] = 10-8 -10-1 M) and rates were measured for 13X and 4A zeolites and TP-207 and TP-260 organic exchange resins in batch equilibrium and fixed-bed exchange experiments, respectively. At solutions equilibrated with CO2 at 1.0 atm (pH = 3.9), H+ exchange capacities for the materials were similar (1.7-2.4 mmol H+ /g material) and resulted in pH increases from 3.9 to greater than 8.0. Multi-component mixtures using Ca2+ and Mg2+ cations (at 10-3 -10-1 M) in CO2-saturated water were used to probe competitive ion exchange. The presence of divalent cations in solution inhibited H+ exchange, reducing capacities to as low as 0.2 mmol H+ /g for both resins and zeolites. Dynamic H+ exchange capacities in fixed-bed ion exchange columns were similar-to equilibrium values for resins (~1.5 mmol/g) and zeolites (~0.8 mmol/g) using inlet solutions that were equilibrated with gaseous streams of CO2 at 1.0 atm. For the four ion exchange materials studied (e.g., ion exchange resins and synthetic zeolites), quasi-chemical linear driving-force approximations that are in first order in solid-phase capacity, effectively model contaminant breakthrough curves. Experimentally determined rate parameters reflect those determined from pore diffusion with pellets: 0.091 s-1 for R-1, 0.06 s-1 for R-2, 0.04 s-1 for Z-1, and 0.025 s-1 for Z-2, particles larger than 500 µm. Predictive H + titration capacities for these ion exchange materials were within 5% difference of experimentally determined H+ titration capacities: 0.81 mmol H+ g-1 of R-1, 0.68 mmol H+ g-1 of R-2, 0.26 mmol H+ g-1 of Z-1, and 0.18 mmol H+ g-1 of Z-2 for pCO2 = 0.12 atm equilibrated inlet streams. These studies demonstrate that linear driving-force approximations can model experimentally determined H+ removal parameters. Additionally, experimental calcite precipitation from mixing the alkaline CO32- -rich water solution obtained from the ion-exchange column with a synthetic liquid waste stream solution achieved thermodynamic maximum yields.Geochemical and process modeling software was used to identify thermodynamically optimum conditions and to quantify the energy intensity and CO2 reduction potential of a process that sequesters CO2 (dissolved in wastewater) as solid calcium carbonate (CaCO3). CaCO3 yields are maximized when initial calcium to CO2 ratios in the aqueous phase are 1:1. The energy intensity for the ion exchange process (0.22 - 2.10 Megawatt-hour per tonne of CO2 removed (MWh/tCO2)) is dependent upon the concentration of CO2 in the gas phase (i.e., 5-50 vol%) and the produced water composition, with nanofiltration and reverse osmosis steps used to recover magnesium and sodium ions contributing the largest energy requirements (0.07 - 0.80 MWh per t-CO2 removed). Energy consumption was minimized under conditions where CaCO3 yields were maximized for all produced water compositions and CO2 concentrations. The ratio of net CO2 to gross CO2 removal for the process ranged from 0.05 to 0.90, indicating a net CO2 reduction across all conditions studied.Furthermore, this ion exchange process was scaled up to treat 300 L of produced water brine (oiland gas-associated wastewater) per day for CO2 mineralization. Produced water brines are optimal for this process because these brines are (Mg2+, Ca2+)-rich, suitable for CO2 mineralization, and Na+ -rich, optimal for regeneration of the spent ion exchange solids used to induce a pH swing. Proton titration capacities were quantified for aqueous streams in equilibrium with gas streams at various concentrations of CO2 (pCO2 = 0.03 - 0.20 atm; 0.10 - 0.81 mmol H+ per g ion exchange solid) and at various flow rates (0.5 - 2.0 L min-1 ; in equilibrium with 0.12 atm gas phase CO2; 0.65 mmol H+ per g ion exchange solid). Utilizing inlet CO2 concentration at 0.12 atm, 0.5 - 3.5 g CaCO3 per L produced water was precipitated, resulting in energy intensities between 30 - 65 kWh per tonne of CO2 sequestered from pumping and effluent mixing. The energy intensity of the process was dependent on volume ratios of the higher alkaline, ion-exchanged CO2 stream and alkaline cation-rich produced water used to precipitate CaCO3. Thermodynamic simulations for precipitated CaCO3 formation were validated through this system, with calcite as the primary precipitated CaCO3 phase (97%) and 3% FeO solids from produced water. A life cycle assessment was performed to analyze the net carbon emissions of the technology for two produced water compositions in equilibrium with gas streams at various CO2 partial pressures (pCO2 = 0.03 - 0.20 atm) which indicated a net CO2 reduction for pCO2 ≥ 0.12 atm (-0.06 to -0.39 kg CO2e per kg precipitated CaCO3) utilizing calcium-rich brines. The results from this study indicate the ion exchange process can be used to provide alkalinity for the precipitation of carbonate solids for most of the CO2 concentrations, thereby opening a pathway toward sustainable and economic mineralization processes.
일반주제명  
Chemical engineering.
일반주제명  
Industrial engineering.
일반주제명  
Mineralogy.
키워드  
Calcium carbonate
키워드  
Carbon dioxide
키워드  
Energy
키워드  
Ion exchange
키워드  
Mineralization
기타저자  
University of California, Los Angeles Chemical Engineering 0294
기본자료저록  
Dissertations Abstracts International. 85-04B.
기본자료저록  
Dissertation Abstract International
전자적 위치 및 접속  
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■020    ▼a9798380598378
■035    ▼a(MiAaPQ)AAI30690632
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a660
■1001  ▼aBustillos,  Steven  Juan.
■24510▼aImplementation  of  Ion  Exchange  Processes  on  Industrial  Waste  Streams  for  Carbon  Dioxide  Mineralization▼h[electronic  resource]
■260    ▼a[S.l.]:▼bUniversity  of  California,  Los  Angeles.  ▼c2023
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2023
■300    ▼a1  online  resource(142  p.)
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  85-04,  Section:  B.
■500    ▼aAdvisor:  Simonetti,  Dante  A.
■5021  ▼aThesis  (Ph.D.)--University  of  California,  Los  Angeles,  2023.
■506    ▼aThis  item  must  not  be  sold  to  any  third  party  vendors.
■520    ▼aSequestration  of  CO2  within  stable  mineral  carbonates  (e.g.,  CaCO3)  represents  an  attractive  emission  reduction  strategy  as  it  offers  a  leakage-free  alternative  to  geological  storage  of  CO2  in  an  environmentally  benign  form.  However,  the  pH  of  aqueous  streams  equilibrated  with  gaseous  streams  containing  CO2  (pH    8).  Traditionally,  alkalinity  is  provided  by  a  stoichiometric  reagent  (e.g.,  NaOH)  which  renders  these  processes  environmentally  hazardous  and  economically  unfeasible.  This  work  investigates  the  use  of  regenerable  ion-exchange  materials  to  induce  alkalinity  in  CO2-  saturated  aqueous  solutions  such  that  the  pH  shift  required  for  mineralization  occurs  without  the  need  for  stoichiometric  reagents.  Na+  -H+  exchange  isotherms  (at  [H+  ]  =  10-8  -10-1  M)  and  rates  were  measured  for  13X  and  4A  zeolites  and  TP-207  and  TP-260  organic  exchange  resins  in  batch  equilibrium  and  fixed-bed  exchange  experiments,  respectively.  At  solutions  equilibrated  with  CO2  at  1.0  atm  (pH  =  3.9),  H+  exchange  capacities  for  the  materials  were  similar  (1.7-2.4  mmol  H+  /g  material)  and  resulted  in  pH  increases  from  3.9  to  greater  than  8.0.  Multi-component  mixtures  using  Ca2+  and  Mg2+  cations  (at  10-3  -10-1  M)  in  CO2-saturated  water  were  used  to  probe  competitive  ion  exchange.  The  presence  of  divalent  cations  in  solution  inhibited  H+  exchange,  reducing  capacities  to  as  low  as  0.2  mmol  H+  /g  for  both  resins  and  zeolites.  Dynamic  H+  exchange  capacities  in  fixed-bed  ion  exchange  columns  were  similar-to  equilibrium  values  for  resins  (~1.5  mmol/g)  and  zeolites  (~0.8  mmol/g)  using  inlet  solutions  that  were  equilibrated  with  gaseous  streams  of  CO2  at  1.0  atm.  For  the  four  ion  exchange  materials  studied  (e.g.,  ion  exchange  resins  and  synthetic  zeolites),  quasi-chemical  linear  driving-force  approximations  that  are  in  first  order  in  solid-phase  capacity,  effectively  model  contaminant  breakthrough  curves.  Experimentally  determined  rate  parameters  reflect  those  determined  from  pore  diffusion  with  pellets:  0.091  s-1  for  R-1,  0.06  s-1  for  R-2,  0.04  s-1  for  Z-1,  and  0.025  s-1  for  Z-2,  particles  larger  than  500  µm.  Predictive  H  +  titration  capacities  for  these  ion  exchange  materials  were  within  5%  difference  of  experimentally  determined  H+  titration  capacities:  0.81  mmol  H+  g-1  of  R-1,  0.68  mmol  H+  g-1  of  R-2,  0.26  mmol  H+  g-1  of  Z-1,  and  0.18  mmol  H+  g-1  of  Z-2  for  pCO2  =  0.12  atm  equilibrated  inlet  streams.  These  studies  demonstrate  that  linear  driving-force  approximations  can  model  experimentally  determined  H+  removal  parameters.  Additionally,  experimental  calcite  precipitation  from  mixing  the  alkaline  CO32-  -rich  water  solution  obtained  from  the  ion-exchange  column  with  a  synthetic  liquid  waste  stream  solution  achieved  thermodynamic  maximum  yields.Geochemical  and  process  modeling  software  was  used  to  identify  thermodynamically  optimum  conditions  and  to  quantify  the  energy  intensity  and  CO2  reduction  potential  of  a  process  that  sequesters  CO2  (dissolved  in  wastewater)  as  solid  calcium  carbonate  (CaCO3).  CaCO3  yields  are  maximized  when  initial  calcium  to  CO2  ratios  in  the  aqueous  phase  are  1:1.  The  energy  intensity for  the  ion  exchange  process  (0.22  -  2.10  Megawatt-hour  per  tonne  of  CO2  removed  (MWh/tCO2))  is  dependent  upon  the  concentration  of  CO2  in  the  gas  phase  (i.e.,  5-50  vol%)  and  the  produced  water  composition,  with  nanofiltration  and  reverse  osmosis  steps  used  to  recover  magnesium  and  sodium  ions  contributing  the  largest  energy  requirements  (0.07  -  0.80  MWh  per  t-CO2  removed).  Energy  consumption  was  minimized  under  conditions  where  CaCO3  yields  were  maximized  for  all  produced  water  compositions  and  CO2  concentrations.  The  ratio  of  net  CO2  to  gross  CO2  removal  for  the  process  ranged  from  0.05  to  0.90,  indicating  a  net  CO2  reduction  across  all  conditions  studied.Furthermore,  this  ion  exchange  process  was  scaled  up  to  treat  300  L  of  produced  water  brine  (oiland  gas-associated  wastewater)  per  day  for  CO2  mineralization.  Produced  water  brines  are  optimal  for  this  process  because  these  brines  are  (Mg2+,  Ca2+)-rich,  suitable  for  CO2  mineralization,  and  Na+  -rich,  optimal  for  regeneration  of  the  spent  ion  exchange  solids  used  to  induce  a  pH  swing.  Proton  titration  capacities  were  quantified  for  aqueous  streams  in  equilibrium  with  gas  streams  at  various  concentrations  of  CO2  (pCO2  =  0.03  -  0.20  atm;  0.10  -  0.81  mmol  H+  per  g  ion  exchange  solid)  and  at  various  flow  rates  (0.5  -  2.0  L  min-1  ;  in  equilibrium  with  0.12  atm  gas  phase  CO2;  0.65  mmol  H+  per  g  ion  exchange  solid).  Utilizing  inlet  CO2  concentration  at  0.12  atm,  0.5  -  3.5  g  CaCO3  per  L  produced  water  was  precipitated,  resulting  in  energy  intensities  between  30  -  65  kWh  per  tonne  of  CO2  sequestered  from  pumping  and  effluent  mixing.  The  energy  intensity  of  the  process  was  dependent  on  volume  ratios  of  the  higher  alkaline,  ion-exchanged  CO2  stream  and  alkaline  cation-rich  produced  water  used  to  precipitate  CaCO3.  Thermodynamic  simulations  for  precipitated  CaCO3  formation  were  validated  through  this  system,  with  calcite  as  the  primary  precipitated  CaCO3  phase  (97%)  and  3%  FeO  solids  from  produced  water.  A  life  cycle assessment  was  performed  to  analyze  the  net  carbon  emissions  of  the  technology  for  two  produced  water  compositions  in  equilibrium  with  gas  streams  at  various  CO2  partial  pressures  (pCO2  =  0.03  -  0.20  atm)  which  indicated  a  net  CO2  reduction  for  pCO2  ≥  0.12  atm  (-0.06  to  -0.39  kg  CO2e  per  kg  precipitated  CaCO3)  utilizing  calcium-rich  brines.  The  results  from  this  study  indicate  the  ion  exchange  process  can  be  used  to  provide  alkalinity  for  the  precipitation  of  carbonate  solids  for  most  of  the  CO2  concentrations,  thereby  opening  a  pathway  toward  sustainable  and  economic  mineralization  processes.
■590    ▼aSchool  code:  0031.
■650  4▼aChemical  engineering.
■650  4▼aIndustrial  engineering.
■650  4▼aMineralogy.
■653    ▼aCalcium  carbonate
■653    ▼aCarbon  dioxide
■653    ▼aEnergy
■653    ▼aIon  exchange
■653    ▼aMineralization
■690    ▼a0542
■690    ▼a0411
■690    ▼a0546
■71020▼aUniversity  of  California,  Los  Angeles▼bChemical  Engineering  0294.
■7730  ▼tDissertations  Abstracts  International▼g85-04B.
■773    ▼tDissertation  Abstract  International
■790    ▼a0031
■791    ▼aPh.D.
■792    ▼a2023
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T16935947▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.
■980    ▼a202402▼f2024

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