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Constraining Sources of Archaeal Tetra-Ether Lipids in Marine Sediments Using Compound-Specific Isotope Analysis
Constraining Sources of Archaeal Tetra-Ether Lipids in Marine Sediments Using Compound-Spe...
Constraining Sources of Archaeal Tetra-Ether Lipids in Marine Sediments Using Compound-Specific Isotope Analysis

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20250211152832
ISBN  
9798346532774
DDC  
551
저자명  
Keller, Katherine.
서명/저자  
Constraining Sources of Archaeal Tetra-Ether Lipids in Marine Sediments Using Compound-Specific Isotope Analysis
발행사항  
[Sl] : Harvard University, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
111 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-05, Section: B.
주기사항  
Advisor: Pearson, Ann.
학위논문주기  
Thesis (Ph.D.)--Harvard University, 2024.
초록/해제  
요약Archaeal isoprenoid glycerol dialkyl glycerol tetraether lipids (iGDGTs) are commonly used tools in paleooceanography for reconstructing past surface temperatures and carbon cycle dynamics. However, uncertainties persist regarding the origins of iGDGTs in marine sediments, requiring a deeper understanding of their diverse sources. The TEX86 sea-surface temperature proxy, based on the ratio of cyclized iGDGTs, assumes that majority of sedimentary iGDGTs originate from a single, planktonic archaeal representative. Yet, the influence of allochthonous input from benthic in-situ and terrestrial sources is unresolved, potentially calling into question the fidelity of iGDGT-based proxies. This thesis aims to address these uncertainties by constraining sources of sedimentary iGDGTs through compound-specific carbon and hydrogen isotope analysis. We develop a dual-isotopic framework to determine iGDGT source apportionment in methane-impacted systems, characterize the δ13C and δ2H isotopic signatures and lipid profiles of potential archaeal sources, and evaluate the impact of heterogenous inputs on the reliability and application of iGDGT-based proxies.In Chapter 2, we conducted analytical tests to evaluate the effects of high-performance liquid chromatography (HPLC) on the carbon isotopic (δ13C) analysis of iGDGTs. Our findings show that normal phase HPLC can cause significant isotopic fractionation, exceeding analytical thresholds, emphasizing the need for precise and complete peak collection during normal phase HPLC for accurate isotope ratio quantification. In Chapter 3, we measured the δ13C values and relative lipid abundances of iGDGTs from three cold-seep locations along Cascadia Margin, using a Bayesian mixing model to robustly characterize the δ13C signatures, lipid profiles and relative contributions to the marine sediment of three potential archaeal endmembers. Our results indicate that the cold seep systems in this region can be described as a binary mixing system between planktonic and benthic-methane cycling archaeal groups, with minimal contribution from benthic non-methane-cycling archaea. Finally, in Chapter 4, we introduce a novel dual-isotope approach, combining δ2H and δ13C analyses of biphytanes derivatives and parent iGDGTs, respectively, to quantitatively distinguish lipid inputs to marine systems. Our findings indicate that planktonic and benthic methane-cycling archaea both yield highly 2H-fractionated lipids, providing an interpretative basis for applying dual isotopic analysis to disentangle iGDGT sources in marine systems.
일반주제명  
Biogeochemistry
일반주제명  
Geochemistry
일반주제명  
Sedimentary geology
일반주제명  
Marine geology
일반주제명  
Analytical chemistry
키워드  
Archaeal tetra-ether lipids
키워드  
Isotopes
키워드  
Lipid biomarkers
키워드  
Marine sediments
키워드  
High-performance liquid chromatography
기타저자  
Harvard University Earth and Planetary Sciences
기본자료저록  
Dissertations Abstracts International. 86-05B.
전자적 위치 및 접속  
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MARC

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■0820  ▼a551
■1001  ▼aKeller,  Katherine.▼0(orcid)0000-0001-6915-5455
■24510▼aConstraining  Sources  of  Archaeal  Tetra-Ether  Lipids  in  Marine  Sediments  Using  Compound-Specific  Isotope  Analysis
■260    ▼a[Sl]▼bHarvard  University▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a111  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-05,  Section:  B.
■500    ▼aAdvisor:  Pearson,  Ann.
■5021  ▼aThesis  (Ph.D.)--Harvard  University,  2024.
■520    ▼aArchaeal  isoprenoid  glycerol  dialkyl  glycerol  tetraether  lipids  (iGDGTs)  are  commonly  used  tools  in  paleooceanography  for  reconstructing  past  surface  temperatures  and  carbon  cycle  dynamics.  However,  uncertainties  persist  regarding  the  origins  of  iGDGTs  in  marine  sediments,  requiring  a  deeper  understanding  of  their  diverse  sources.  The  TEX86  sea-surface  temperature  proxy,  based  on  the  ratio  of  cyclized  iGDGTs,  assumes  that  majority  of  sedimentary  iGDGTs  originate  from  a  single,  planktonic  archaeal  representative.  Yet,  the  influence  of  allochthonous  input  from  benthic  in-situ  and  terrestrial  sources  is  unresolved,  potentially  calling  into  question  the  fidelity  of  iGDGT-based  proxies.  This  thesis  aims  to  address  these  uncertainties  by  constraining  sources  of  sedimentary  iGDGTs  through  compound-specific  carbon  and  hydrogen  isotope  analysis.  We  develop  a  dual-isotopic  framework  to  determine  iGDGT  source  apportionment  in  methane-impacted  systems,  characterize  the  δ13C  and  δ2H  isotopic  signatures  and  lipid  profiles  of  potential  archaeal  sources,  and  evaluate  the  impact  of  heterogenous  inputs  on  the  reliability  and  application  of  iGDGT-based  proxies.In  Chapter  2,  we  conducted  analytical  tests  to  evaluate  the  effects  of  high-performance  liquid  chromatography  (HPLC)  on  the  carbon  isotopic  (δ13C)  analysis  of  iGDGTs.  Our  findings  show  that  normal  phase  HPLC  can  cause  significant  isotopic  fractionation,  exceeding  analytical  thresholds,  emphasizing  the  need  for  precise  and  complete  peak  collection  during  normal  phase  HPLC  for  accurate  isotope  ratio  quantification.  In  Chapter  3,  we  measured  the  δ13C  values  and  relative  lipid  abundances  of  iGDGTs  from  three  cold-seep  locations  along  Cascadia  Margin,  using  a  Bayesian  mixing  model  to  robustly  characterize  the  δ13C  signatures,  lipid  profiles  and  relative  contributions  to  the  marine  sediment  of  three  potential  archaeal  endmembers.  Our  results  indicate  that  the  cold  seep  systems  in  this  region  can  be  described  as  a  binary  mixing  system  between  planktonic  and  benthic-methane  cycling  archaeal  groups,  with  minimal  contribution  from  benthic  non-methane-cycling  archaea.  Finally,  in  Chapter  4,  we  introduce  a  novel  dual-isotope  approach,  combining  δ2H  and  δ13C  analyses  of  biphytanes  derivatives  and  parent  iGDGTs,  respectively,  to  quantitatively  distinguish  lipid  inputs  to  marine  systems.  Our  findings  indicate  that  planktonic  and  benthic  methane-cycling  archaea  both  yield  highly  2H-fractionated  lipids,  providing  an  interpretative  basis  for  applying  dual  isotopic  analysis  to  disentangle  iGDGT  sources  in  marine  systems.
■590    ▼aSchool  code:  0084.
■650  4▼aBiogeochemistry
■650  4▼aGeochemistry
■650  4▼aSedimentary  geology
■650  4▼aMarine  geology
■650  4▼aAnalytical  chemistry
■653    ▼aArchaeal  tetra-ether  lipids
■653    ▼aIsotopes
■653    ▼aLipid  biomarkers
■653    ▼aMarine  sediments
■653    ▼aHigh-performance  liquid  chromatography
■690    ▼a0425
■690    ▼a0996
■690    ▼a0486
■690    ▼a0556
■690    ▼a0594
■71020▼aHarvard  University▼bEarth  and  Planetary  Sciences.
■7730  ▼tDissertations  Abstracts  International▼g86-05B.
■790    ▼a0084
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17164102▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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