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Nanopatterned Electrochemical Biosensor Electrodes With Enhanced Signal and Sensitivity
Nanopatterned Electrochemical Biosensor Electrodes With Enhanced Signal and Sensitivity
Nanopatterned Electrochemical Biosensor Electrodes With Enhanced Signal and Sensitivity

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자료유형  
 학위논문 서양
최종처리일시  
20250211151019
ISBN  
9798383482292
DDC  
620.11
저자명  
Kinser, Emily R.
서명/저자  
Nanopatterned Electrochemical Biosensor Electrodes With Enhanced Signal and Sensitivity
발행사항  
[Sl] : Yale University, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
227 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-01, Section: B.
주기사항  
Advisor: Kyriakides, Themis;Schroers, Jan.
학위논문주기  
Thesis (Ph.D.)--Yale University, 2024.
초록/해제  
요약Innovations in materials and process development in recent decades have enabled surface engineering at the nanoscale, which provides a pathway to improvement in the performance and longevity of biomedical implants and biosensors. One such novel class of materials is bulk metallic glass. As an amorphous metal, bulk metallic glass can be molded with after initial casting to produce high-precision features by elevating the material above the glass transition temperature, Tg, via the process of thermoplastic forming (TPF). Thus, BMGs enable a unique pathway to molding nano-scale structures in air at comparably low processing temperatures. Platinum-base BMG alloys (Pt-BMGs) are of particular interest for potential use as biomaterials. Nanopatterned Pt-BMG substrates with arrays of nanorods ranging from 55 nm - 200 nm in nominal diameter were fabricated using TPF, and the interaction of several different cell types associated with FBR with the nanopatterned Pt-BMG substrates was evaluated. The Pt-BMG alloy was determined to be biocompatible, and the response to the range of nanotopographies differed by cell type. For all cell types, the cells demonstrated the ability to sense and respond to the nanotopography, which influenced cell function and morphology.Nanopattern-cell interactions for fibroblast cells on Pt-BMG substrates were investigated using FIB-SEM; this revealed a mechanosensing mechanism of the cells which was associated with nanorod bending across the cell radius. Analysis of cellular traction force showed how varying the mechanical properties and design of the nanotopography on a surface can influence cell behavior. Nanorod bending near the cell perimeter was confirmed by examining live fibroblast cells with intact cell membranes using confocal microscopy with reflectance of the nanorods in order to concurrently image the nanopattern-cell interaction at both the micro- and nano-scales.Nanopatterned Pt-BMGs were also identified as potential electrode architecture for electrochemical biosensing applications due to the PT-BMG alloy's chemistry combined with the increase in electrode surface area associated with the nanorods. Glucose was selected as the target biological molecule, and Pt-BMG substrates nanopatterned with 200 nm diameter nanorods were functionalized with glucose oxidase enzyme to be utilized as biosensor electrodes. The Pt-BMG electrodes were successfully demonstrated to function as electrochemical glucose biosensors. In order to assess the impact of electrode surface area on sensor performance, two nanotopographies were evaluated: 200 nm Pt-BMG arrays fabricated using the same protocol as the prior cell study (25 kN applied force during TPF), and a second 200 nm Pt-BMG nanopattern which were created using a lower applied force during TPF (7 KN) in order to produce nanorods with reduced height. When compared to a flat Pt-BMG control, the nanopatterned electrodes both exhibited an increase in sensor electrical signal and sensitivity. The Pt-BMG electrodes with the taller nanorods - and therefore greater surface area - demonstrated an order of magnitude increase in sensitivity. The nanopatterned electrodes with shorter nanorods also resulted in more than three times the sensitivity compared to the flat control. Nanopatterned biosensor electrodes with optimized sensor performance and biocompatibility were next pursued to expand upon the initial demonstration of Pt-BMG nanopatterned biosensor electrodes. By transitioning from TPF of Pt-BMGs for fabricating nanopatterned electrodes to using materials and processes that are used for semiconductor manufacturing, the precision of the nanotopography was improved while also scaling up the electrode size. The transition to semiconductor-compatible processing also enabled agility in the nanopattern design, and arrays of nanorods oriented with different center-to-center spacing were designed in order to assess the impact of nanorod pitch on sensor performance. The nanorod composition and architecture were also re-engineered to enhance electrochemical sensing capability. A hybrid nanorod structure consisting of an electroplated gold core encapsulated by a thin platinum film enabled reliable electrochemical detection with improved electrical signal using biocompatible materials. Cell-nanopattern interaction was again evaluated using fibroblast cells.The hybrid gold-platinum nanopatterned electrodes were demonstrated to successfully detect glucose with greater signal and sensitivity compared to an unpatterned platinum control electrode. Nanorod spacing was also observed to impact sensor performance; the optimal sensor performance was found to be dependent on nanorod density in addition to total effective surface area. When normalized for effective surface area, the performance of the hybrid gold-platinum nanorods exceeded that of the nanopatterned Pt-BMG electrodes for both sensor signal and sensitivity.
일반주제명  
Materials science
키워드  
Biosensor
키워드  
Metallic Glass
키워드  
Nanotopography
기타저자  
Yale University Mechanical Engineering and Materials Science
기본자료저록  
Dissertations Abstracts International. 86-01B.
전자적 위치 및 접속  
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MARC

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■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a620.11
■1001  ▼aKinser,  Emily  R.
■24510▼aNanopatterned  Electrochemical  Biosensor  Electrodes  With  Enhanced  Signal  and  Sensitivity
■260    ▼a[Sl]▼bYale  University▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a227  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-01,  Section:  B.
■500    ▼aAdvisor:  Kyriakides,  Themis;Schroers,  Jan.
■5021  ▼aThesis  (Ph.D.)--Yale  University,  2024.
■520    ▼aInnovations  in  materials  and  process  development  in  recent  decades  have  enabled  surface  engineering  at  the  nanoscale,  which  provides  a  pathway  to  improvement  in  the  performance  and  longevity  of  biomedical  implants  and  biosensors.  One  such  novel  class  of  materials  is  bulk  metallic  glass.  As  an  amorphous  metal,  bulk  metallic  glass  can  be  molded  with  after  initial  casting  to  produce  high-precision  features  by  elevating  the  material  above  the  glass  transition  temperature,  Tg,  via  the  process  of  thermoplastic  forming  (TPF).  Thus,  BMGs  enable  a  unique  pathway  to  molding  nano-scale  structures  in  air  at  comparably  low  processing  temperatures.  Platinum-base  BMG  alloys  (Pt-BMGs)  are  of  particular  interest  for  potential  use  as  biomaterials.  Nanopatterned  Pt-BMG  substrates  with  arrays  of  nanorods  ranging  from  55  nm  -  200  nm  in  nominal  diameter  were  fabricated  using  TPF,  and  the  interaction  of  several  different  cell  types  associated  with  FBR  with  the  nanopatterned  Pt-BMG  substrates  was  evaluated.  The  Pt-BMG  alloy  was  determined  to  be  biocompatible,  and  the  response  to  the  range  of  nanotopographies  differed  by  cell  type.  For  all  cell  types,  the  cells  demonstrated  the  ability  to  sense  and  respond  to  the  nanotopography,  which  influenced  cell  function  and  morphology.Nanopattern-cell  interactions  for  fibroblast  cells  on  Pt-BMG  substrates  were  investigated  using  FIB-SEM;  this  revealed  a  mechanosensing  mechanism  of  the  cells  which  was  associated  with  nanorod  bending  across  the  cell  radius.  Analysis  of  cellular  traction  force  showed  how  varying  the  mechanical  properties  and  design  of  the  nanotopography  on  a  surface  can  influence  cell  behavior.  Nanorod  bending  near  the  cell  perimeter  was  confirmed  by  examining  live  fibroblast  cells  with  intact  cell  membranes  using  confocal  microscopy  with  reflectance  of  the  nanorods  in  order  to  concurrently  image  the  nanopattern-cell  interaction  at  both  the  micro-  and  nano-scales.Nanopatterned  Pt-BMGs  were  also  identified  as  potential  electrode  architecture  for  electrochemical  biosensing  applications  due  to  the  PT-BMG  alloy's  chemistry  combined  with  the  increase  in  electrode  surface  area  associated  with  the  nanorods.  Glucose  was  selected  as  the  target  biological  molecule,  and  Pt-BMG  substrates  nanopatterned  with  200  nm  diameter  nanorods  were  functionalized  with  glucose  oxidase  enzyme  to  be  utilized  as  biosensor  electrodes.  The  Pt-BMG  electrodes  were  successfully  demonstrated  to  function  as  electrochemical  glucose  biosensors.  In  order  to  assess  the  impact  of  electrode  surface  area  on  sensor  performance,  two  nanotopographies  were  evaluated:  200  nm  Pt-BMG  arrays  fabricated  using  the  same  protocol  as  the  prior  cell  study  (25  kN  applied  force  during  TPF),  and  a  second  200  nm  Pt-BMG  nanopattern  which  were  created  using  a  lower  applied  force  during  TPF  (7  KN)  in  order  to  produce  nanorods  with  reduced  height.  When  compared  to  a  flat  Pt-BMG  control,  the  nanopatterned  electrodes  both  exhibited  an  increase  in  sensor  electrical  signal  and  sensitivity.  The  Pt-BMG  electrodes  with  the  taller  nanorods  -  and  therefore  greater  surface  area  -  demonstrated  an  order  of  magnitude  increase  in  sensitivity.  The  nanopatterned  electrodes  with  shorter  nanorods  also  resulted  in  more  than  three  times  the  sensitivity  compared  to  the  flat  control.  Nanopatterned  biosensor  electrodes  with  optimized  sensor  performance  and  biocompatibility  were  next  pursued  to  expand  upon  the  initial  demonstration  of  Pt-BMG  nanopatterned  biosensor  electrodes.  By  transitioning  from  TPF  of  Pt-BMGs  for  fabricating  nanopatterned  electrodes  to  using  materials  and  processes  that  are  used  for  semiconductor  manufacturing,  the  precision  of  the  nanotopography  was  improved  while  also  scaling  up  the  electrode  size.  The  transition  to  semiconductor-compatible  processing  also  enabled  agility  in  the  nanopattern  design,  and  arrays  of  nanorods  oriented  with  different  center-to-center  spacing  were  designed  in  order  to  assess  the  impact  of  nanorod  pitch  on  sensor  performance.  The  nanorod  composition  and  architecture  were  also  re-engineered  to  enhance  electrochemical  sensing  capability.  A  hybrid  nanorod  structure  consisting  of  an  electroplated  gold  core  encapsulated  by  a  thin  platinum  film  enabled  reliable  electrochemical  detection  with  improved  electrical  signal  using  biocompatible  materials.  Cell-nanopattern  interaction  was  again  evaluated  using  fibroblast  cells.The  hybrid  gold-platinum  nanopatterned  electrodes  were  demonstrated  to  successfully  detect  glucose  with  greater  signal  and  sensitivity  compared  to  an  unpatterned  platinum  control  electrode.  Nanorod  spacing  was  also  observed  to  impact  sensor  performance;  the  optimal  sensor  performance  was  found  to  be  dependent  on  nanorod  density  in  addition  to  total  effective  surface  area.  When  normalized  for  effective  surface  area,  the  performance  of  the  hybrid  gold-platinum  nanorods  exceeded  that  of  the  nanopatterned  Pt-BMG  electrodes  for  both  sensor  signal  and  sensitivity.
■590    ▼aSchool  code:  0265.
■650  4▼aMaterials  science
■653    ▼aBiosensor
■653    ▼aMetallic  Glass
■653    ▼aNanotopography
■690    ▼a0794
■71020▼aYale  University▼bMechanical  Engineering  and  Materials  Science.
■7730  ▼tDissertations  Abstracts  International▼g86-01B.
■790    ▼a0265
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17160440▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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