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Use of Organic Bases in the Synthesis of Geopolymers
Use of Organic Bases in the Synthesis of Geopolymers
Use of Organic Bases in the Synthesis of Geopolymers

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자료유형  
 학위논문 서양
최종처리일시  
20260202105703
ISBN  
9798263308087
DDC  
620.11
저자명  
Samuel, Devon.
서명/저자  
Use of Organic Bases in the Synthesis of Geopolymers
발행사항  
[Sl] : University of Illinois at Urbana-Champaign, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
241 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-05, Section: B.
주기사항  
Advisor: Kriven, Waltraud M.
학위논문주기  
Thesis (Ph.D.)--University of Illinois at Urbana-Champaign, 2024.
초록/해제  
요약Alkali geopolymers are a facile forming route for alkali aluminosilicate ceramics because they are formed as fluids and crystallize upon heating to about 1000 °C. It is also possible to replace the alkali cations by an ion exchange process, expanding the number of ceramic compositions that can be made while taking advantage of the versatility in forming afforded by geopolymers. However, the ion exchange process is very slow for small bodies and entirely impractical for pieces thicker than a few millimeters. This thesis investigated the synthesis of geopolymers with organic bases rather than inorganic alkali hydroxides. This would avoid the use of alkali cations entirely and greatly widen the range of ceramics formable via geopolymers. Three organic bases were tested - guanidine, 1,1,3,3-tetramethylguanidine (TMG), and tetramethylammonium hydroxide (TMAOH) - for their ability to form geopolymers with Al2O3:SiO2 ratios of 1:2 and 1:4 as well as 3:2 to match the composition of mullite, a common ceramic. Guanidine was successful, causing reaction at room temperature and producing bodies with atomic structures and microstructures similar to the equivalent sodium geopolymer compositions. TMAOH was able to induce setting in Al2O3•4 SiO2 systems, but they required heating to 50 °C for 1 month, and the resultant bodies were substantially different from sodium geopolymers. An even higher cure temperature, such as 80 °C, might reduce the setting time and improve the reaction into a geopolymeric material. TMG was entirely unsuccessful, and no compositions solidified or even exhibited a substantial extent of reaction. For the organic base compositions that solidified, their crystallization upon heating was studied up to 1600 °C. The Al2O3•2 SiO2 and Al2O3•4 SiO2 compositions produced mullite + glass and the 3 Al2O3•2 SiO2 compositions became almost pure mullite. All of them had substantial amounts of porosity after firing from a combination of the geopolymer synthesis method and the firing program. The amount of porosity and crystal morphology varied with the organic base, overall composition, and choice of precursors used to reach the 3 Al2O3•2 SiO2 composition. An alternative route to casting a pre-mullite material was devised which relied only on having a solution with high pH and an amorphous mullite powder with a high fraction of five-coordinated aluminum. These compositions behaved like hydratable alumina binders and were bound together by precipitated aluminum hydroxide phases rather than geopolymer. However, it seemed to be more generally viable and all of the organic bases, including TMG, caused setting in a short time, albeit with some differences in the microstructure and density after firing. Attempts to extend this method to non-mullite aluminate compositions, using MgO•Al2O3 and 3 Y2O3•5 Al2O3 as examples, were not successful. Although the use of an alkaline solution instead of water alone did induce a greater degree of aluminum hydroxide precipitation, there was not always enough aluminum hydroxide to bind the material and setting was sometimes delayed rather than accelerated. The use of organic base geopolymers for producing non-mullite ceramics was demonstrated by the synthesis of cordierite (2 MgO•2 Al2O3•5 SiO2) from a guanidine metakaolin-based geopolymer. The field of available ceramics was expanded further by showing that geopolymer-like materials could be made using Y2O3 and ZnO as substitutes for metakaolin, giving Y2O3•2 SiO2 and 2 ZnO•SiO2 compositions, respectively.
일반주제명  
Materials science
일반주제명  
Engineering
키워드  
Geopolymers
키워드  
Organic base
키워드  
Aluminosilicate ceramics
기타저자  
University of Illinois at Urbana-Champaign Materials Science & Engineerng
기본자료저록  
Dissertations Abstracts International. 87-05B.
전자적 위치 및 접속  
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■24510▼aUse  of  Organic  Bases  in  the  Synthesis  of  Geopolymers
■260    ▼a[Sl]▼bUniversity  of  Illinois  at  Urbana-Champaign▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a241  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-05,  Section:  B.
■500    ▼aAdvisor:  Kriven,  Waltraud  M.
■5021  ▼aThesis  (Ph.D.)--University  of  Illinois  at  Urbana-Champaign,  2024.
■520    ▼aAlkali  geopolymers  are  a  facile  forming  route  for  alkali  aluminosilicate  ceramics  because  they  are  formed  as  fluids  and  crystallize  upon  heating  to  about  1000  °C.  It  is  also  possible  to  replace  the  alkali  cations  by  an  ion  exchange  process,  expanding  the  number  of  ceramic  compositions  that  can  be  made  while  taking  advantage  of  the  versatility  in  forming  afforded  by  geopolymers.  However,  the  ion  exchange  process  is  very  slow  for  small  bodies  and  entirely  impractical  for  pieces  thicker  than  a  few  millimeters.                        This  thesis  investigated  the  synthesis  of  geopolymers  with  organic  bases  rather  than  inorganic  alkali  hydroxides.  This  would  avoid  the  use  of  alkali  cations  entirely  and  greatly  widen  the  range  of  ceramics  formable  via  geopolymers.  Three  organic  bases  were  tested  -  guanidine,  1,1,3,3-tetramethylguanidine  (TMG),  and  tetramethylammonium  hydroxide  (TMAOH)  -  for  their  ability  to  form  geopolymers  with  Al2O3:SiO2  ratios  of  1:2  and  1:4  as  well  as  3:2  to  match  the  composition  of  mullite,  a  common  ceramic.  Guanidine  was  successful,  causing  reaction  at  room  temperature  and  producing  bodies  with  atomic  structures  and  microstructures  similar  to  the  equivalent  sodium  geopolymer  compositions.  TMAOH  was  able  to  induce  setting  in  Al2O3•4  SiO2  systems,  but  they  required  heating  to  50  °C  for  1  month,  and  the  resultant  bodies  were  substantially  different  from  sodium  geopolymers.  An  even  higher  cure  temperature,  such  as  80  °C,  might  reduce  the  setting  time  and  improve  the  reaction  into  a  geopolymeric  material.  TMG  was  entirely  unsuccessful,  and  no  compositions  solidified  or  even  exhibited  a  substantial  extent  of  reaction.                        For  the  organic  base  compositions  that  solidified,  their  crystallization  upon  heating  was  studied  up  to  1600  °C.  The  Al2O3•2  SiO2  and  Al2O3•4  SiO2  compositions  produced  mullite  +  glass  and  the  3  Al2O3•2  SiO2  compositions  became  almost  pure  mullite.  All  of  them  had  substantial  amounts  of  porosity  after  firing  from  a  combination  of  the  geopolymer  synthesis  method  and  the  firing  program.  The  amount  of  porosity  and  crystal  morphology  varied  with  the  organic  base,  overall  composition,  and  choice  of  precursors  used  to  reach  the  3  Al2O3•2  SiO2  composition.                        An  alternative  route  to  casting  a  pre-mullite  material  was  devised  which  relied  only  on  having  a  solution  with  high  pH  and  an  amorphous  mullite  powder  with  a  high  fraction  of  five-coordinated  aluminum.  These  compositions  behaved  like  hydratable  alumina  binders  and  were  bound  together  by  precipitated  aluminum  hydroxide  phases  rather  than  geopolymer.  However,  it  seemed  to  be  more  generally  viable  and  all  of  the  organic  bases,  including  TMG,  caused  setting  in  a  short  time,  albeit  with  some  differences  in  the  microstructure  and  density  after  firing.  Attempts  to  extend  this  method  to  non-mullite  aluminate  compositions,  using  MgO•Al2O3  and  3  Y2O3•5  Al2O3  as  examples,  were  not  successful.  Although  the  use  of  an  alkaline  solution  instead  of  water  alone  did  induce  a  greater  degree  of  aluminum  hydroxide  precipitation,  there  was  not  always  enough  aluminum  hydroxide  to  bind  the  material  and  setting  was  sometimes  delayed  rather  than  accelerated.                        The  use  of  organic  base  geopolymers  for  producing  non-mullite  ceramics  was  demonstrated  by  the  synthesis  of  cordierite  (2  MgO•2  Al2O3•5  SiO2)  from  a  guanidine  metakaolin-based  geopolymer.  The  field  of  available  ceramics  was  expanded  further  by  showing  that  geopolymer-like  materials  could  be  made  using  Y2O3  and  ZnO  as  substitutes  for  metakaolin,  giving  Y2O3•2  SiO2  and  2  ZnO•SiO2  compositions,  respectively.
■590    ▼aSchool  code:  0090.
■650  4▼aMaterials  science
■650  4▼aEngineering
■653    ▼aGeopolymers
■653    ▼aOrganic  base
■653    ▼aAluminosilicate  ceramics
■690    ▼a0794
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■71020▼aUniversity  of  Illinois  at  Urbana-Champaign▼bMaterials  Science  &  Engineerng.
■7730  ▼tDissertations  Abstracts  International▼g87-05B.
■790    ▼a0090
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17361085▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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