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Mixture Adsorption in Metal-Organic Frameworks for Biogas and Light Hydrocarbon Separation
Mixture Adsorption in Metal-Organic Frameworks for Biogas and Light Hydrocarbon Separation
Mixture Adsorption in Metal-Organic Frameworks for Biogas and Light Hydrocarbon Separation

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20260202105330
ISBN  
9798263324742
DDC  
363.738
저자명  
Li, Chunyi.
서명/저자  
Mixture Adsorption in Metal-Organic Frameworks for Biogas and Light Hydrocarbon Separation
발행사항  
[Sl] : Georgia Institute of Technology, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
308 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-05, Section: B.
주기사항  
Advisor: Lively, Ryan P.
학위논문주기  
Thesis (Ph.D.)--Georgia Institute of Technology, 2024.
초록/해제  
요약As the global energy demand continues to increase, developing technologies to use renewable energy sources has become increasingly urgent. The development of biogas separation for biomethane production opens possibilities for renewable energy utilization. Biogas is versatile in terms of both production and utilization. It can be used for heat, power, and electricity generation in place of fossil fuels. Additionally, it can be integrated into areas where natural gas is used for vehicular fuel and chemical production. Along with the various biogas sources, numerous challenges are present with effective biogas separation. Biogas contains mainly carbon dioxide and methane, with low concentrations of contaminants such as hydrogen sulfide (H2S) and ammonia (NH3). In municipal landfill biogas, mercaptans and siloxanes are also present in trace amounts. In addition, biogas is saturated with water from the natural fermentation processes. Typical biogas utilization requires pre-drying and desulfurization. Specifically, the H2S concentration needs to be reduced to below 20 parts per million (ppm) for pipeline transportation from starting concentrations of above 3000 ppm.The desulfurization step is typically achieved by biologically oxidizing H2S into elemental sulfur. This process requires air injection and sometimes bacterial introduction. Despite the advantage of desulfurization inside the fermentation chamber, air injection lowers the heating value of biogas by introducing large quantities of nitrogen. Aqueous scrubbing using water or polyethylene glycol solutions faces the problem of producing large amounts of contaminated solutions and high-cost regeneration. Membrane separation is not ideal for desulfurization due to the low driving force from the low concentrations of contaminants. After drying and desulfurization, most of the CO2 is removed to produce higher-heating value biomethane. Adsorption using activated carbon requires low-cost operation, but the relatively low affinity to H2S and CO2 results in low adsorption selectivities over CH4.Much effort has been focused on developing sorbent materials for selective H2S and CO2 separation. There is a need to study the adsorption performance in realistic gas mixtures to understand the competitive adsorption behavior of gases. In this thesis, the mixture adsorption equilibrium of H2S and CO2 was studied using simulated biogas mixtures containing H2S, CO2, methane, and water vapor. The approach of this thesis is summarized in four objectives.The first objective investigates the chemical stability of metal-organic frameworks (MOFs) in H2S and CO2-containing environments. In Chapter 4, the chemical stability and structural stability of MIL-125-NH2 in the presence of dry H2S up is studied using in situ and ex situ characterization methods. In Chapter 6 and Chapter 7, the H2S adsorption performance in diamine-impregnated MIL-101(Cr) is studied in adsorption-desorption cycles using dry and humid simulated biogas mixtures. The effect of the type of diamine on the cyclic adsorption stability of H2S and CO2 is studied using diamines containing 1°,1° amines, 1°,2° amines, and 1°,3° amines. The study concludes that the impregnation of diamine in MIL-101(Cr) improves the cyclic adsorption stability of H2S. The second objective studies the effect of metal substitution on mixture adsorption equilibrium of ethylene and acetylene using isostructural MOFs. The production of ethylene from biomethane may contain trace amounts of acetylene and ethane. Acetylene is also a problematic contaminant in ethylene produced from naphtha cracking. Chapter 5 uses four isostructural MOFs based on rare-earth metals to study the acetylene/ethylene adsorption selectivity. The experimental results show that the pore size decrease across the rare-earth MOFs played a role in determining the acetylene/ethylene selectivity and acetylene adsorption capacity.
일반주제명  
Greenhouse gases
일반주제명  
Alternative energy sources
일반주제명  
Landfill
일반주제명  
Emissions
일반주제명  
Households
일반주제명  
Natural gas
일반주제명  
Alternative energy
일반주제명  
Climate change
일반주제명  
Petroleum engineering
기타저자  
Georgia Institute of Technology.
기본자료저록  
Dissertations Abstracts International. 87-05B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aLi,  Chunyi.
■24510▼aMixture  Adsorption  in  Metal-Organic  Frameworks  for  Biogas  and  Light  Hydrocarbon  Separation
■260    ▼a[Sl]▼bGeorgia  Institute  of  Technology▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a308  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-05,  Section:  B.
■500    ▼aAdvisor:  Lively,  Ryan  P.
■5021  ▼aThesis  (Ph.D.)--Georgia  Institute  of  Technology,  2024.
■520    ▼aAs  the  global  energy  demand  continues  to  increase,  developing  technologies  to  use  renewable  energy  sources  has  become  increasingly  urgent.  The  development  of  biogas  separation  for  biomethane  production  opens  possibilities  for  renewable  energy  utilization.  Biogas  is  versatile  in  terms  of  both  production  and  utilization.  It  can  be  used  for  heat,  power,  and  electricity  generation  in  place  of  fossil  fuels.  Additionally,  it  can  be  integrated  into  areas  where  natural  gas  is  used  for  vehicular  fuel  and  chemical  production.  Along  with  the  various  biogas  sources,  numerous  challenges  are  present  with  effective  biogas  separation.  Biogas  contains  mainly  carbon  dioxide  and  methane,  with  low  concentrations  of  contaminants  such  as  hydrogen  sulfide  (H2S)  and  ammonia  (NH3).  In  municipal  landfill  biogas,  mercaptans  and  siloxanes  are  also  present  in  trace  amounts.  In  addition,  biogas  is  saturated  with  water  from  the  natural  fermentation  processes.  Typical  biogas  utilization  requires  pre-drying  and  desulfurization.  Specifically,  the  H2S  concentration  needs  to  be  reduced  to  below  20  parts  per  million  (ppm)  for  pipeline  transportation  from  starting  concentrations  of  above  3000  ppm.The  desulfurization  step  is  typically  achieved  by  biologically  oxidizing  H2S  into  elemental  sulfur.  This  process  requires  air  injection  and  sometimes  bacterial  introduction.  Despite  the  advantage  of  desulfurization  inside  the  fermentation  chamber,  air  injection  lowers  the  heating  value  of  biogas  by  introducing  large  quantities  of  nitrogen.  Aqueous  scrubbing  using  water  or  polyethylene  glycol  solutions  faces  the  problem  of  producing  large  amounts  of  contaminated  solutions  and  high-cost  regeneration.  Membrane  separation  is  not  ideal  for  desulfurization  due  to  the  low  driving  force  from  the  low  concentrations  of  contaminants.  After  drying  and  desulfurization,  most  of  the  CO2  is  removed  to  produce  higher-heating  value  biomethane.  Adsorption  using  activated  carbon  requires  low-cost  operation,  but  the  relatively  low  affinity  to  H2S  and  CO2  results  in  low  adsorption  selectivities  over  CH4.Much  effort  has  been  focused  on  developing  sorbent  materials  for  selective  H2S  and  CO2  separation.  There  is  a  need  to  study  the  adsorption  performance  in  realistic  gas  mixtures  to  understand  the  competitive  adsorption  behavior  of  gases.  In  this  thesis,  the  mixture  adsorption  equilibrium  of  H2S  and  CO2  was  studied  using  simulated  biogas  mixtures  containing  H2S,  CO2,  methane,  and  water  vapor.  The  approach  of  this  thesis  is  summarized  in  four  objectives.The  first  objective  investigates  the  chemical  stability  of  metal-organic  frameworks  (MOFs)  in  H2S  and  CO2-containing  environments.  In  Chapter  4,  the  chemical  stability  and  structural  stability  of  MIL-125-NH2  in  the  presence  of  dry  H2S  up  is  studied  using  in  situ  and  ex  situ  characterization  methods.  In  Chapter  6  and  Chapter  7,  the  H2S  adsorption  performance  in  diamine-impregnated  MIL-101(Cr)  is  studied  in  adsorption-desorption  cycles  using  dry  and  humid  simulated  biogas  mixtures.  The  effect  of  the  type  of  diamine  on  the  cyclic  adsorption  stability  of  H2S  and  CO2  is  studied  using  diamines  containing  1°,1°  amines,  1°,2°  amines,  and  1°,3°  amines.  The  study  concludes  that  the  impregnation  of  diamine  in  MIL-101(Cr)  improves  the  cyclic  adsorption  stability  of  H2S.  The  second  objective  studies  the  effect  of  metal  substitution  on  mixture  adsorption  equilibrium  of  ethylene  and  acetylene  using  isostructural  MOFs.  The  production  of  ethylene  from  biomethane  may  contain  trace  amounts  of  acetylene  and  ethane.  Acetylene  is  also  a  problematic  contaminant  in  ethylene  produced  from  naphtha  cracking.  Chapter  5  uses  four  isostructural  MOFs  based  on  rare-earth  metals  to  study  the  acetylene/ethylene  adsorption  selectivity.  The  experimental  results  show  that  the  pore  size  decrease  across  the  rare-earth  MOFs  played  a  role  in  determining  the  acetylene/ethylene  selectivity  and  acetylene  adsorption  capacity.
■590    ▼aSchool  code:  0078.
■650  4▼aGreenhouse  gases
■650  4▼aAlternative  energy  sources
■650  4▼aLandfill
■650  4▼aEmissions
■650  4▼aHouseholds
■650  4▼aNatural  gas
■650  4▼aAlternative  energy
■650  4▼aClimate  change
■650  4▼aPetroleum  engineering
■690    ▼a0363
■690    ▼a0404
■690    ▼a0765
■71020▼aGeorgia  Institute  of  Technology.
■7730  ▼tDissertations  Abstracts  International▼g87-05B.
■790    ▼a0078
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17360262▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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