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- Creators: Brahms, Johannes, 1833-1897
Description
Biogenic silica nanostructures, derived from diatoms, possess highly ordered porous hierarchical nanostructures and afford flexibility in design in large part due to the availability of a great variety of shapes, sizes, and symmetries. These advantages have been exploited for study of transport phenomena of ions and molecules towards the goal of developing ultrasensitive and selective filters and biosensors. Diatom frustules give researchers many inspiration and ideas for the design and production of novel nanostructured materials. In this doctoral research will focus on the following three aspects of biogenic silica: 1) Using diatom frustule as protein sensor. 2) Using diatom nanostructures as template to fabricate nano metal materials. 3) Using diatom nanostructures to fabricate hybrid platform.
Nanoscale confinement biogenetic silica template-based electrical biosensor assay offers the user the ability to detect and quantify the biomolecules. Diatoms have been demonstrated as part of a sensor. The sensor works on the principle of electrochemical impedance spectroscopy. When specific protein biomarkers from a test sample bind to corresponding antibodies conjugated to the surface of the gold surface at the base of each nanowell, a perturbation of electrical double layer occurs resulting in a change in the impedance.
Diatoms are also a new source of inspiration for the design and fabrication of nanostructured materials. Template-directed deposition within cylindrical nanopores of a porous membrane represents an attractive and reproducible approach for preparing metal nanopatterns or nanorods of a variety of aspect ratios. The nanopatterns fabricated from diatom have the potential of the metal-enhanced fluorescence to detect dye-conjugated molecules.
Another approach presents a platform integrating biogenic silica nanostructures with micromachined silicon substrates in a micro
ano hybrid device. In this study, one can take advantages of the unique properties of a marine diatom that exhibits nanopores on the order of 40 nm in diameter and a hierarchical structure. This device can be used to several applications, such as nano particles separation and detection. This platform is also a good substrate to study cell growth that one can observe the reaction of cell growing on the nanostructure of frustule.
Nanoscale confinement biogenetic silica template-based electrical biosensor assay offers the user the ability to detect and quantify the biomolecules. Diatoms have been demonstrated as part of a sensor. The sensor works on the principle of electrochemical impedance spectroscopy. When specific protein biomarkers from a test sample bind to corresponding antibodies conjugated to the surface of the gold surface at the base of each nanowell, a perturbation of electrical double layer occurs resulting in a change in the impedance.
Diatoms are also a new source of inspiration for the design and fabrication of nanostructured materials. Template-directed deposition within cylindrical nanopores of a porous membrane represents an attractive and reproducible approach for preparing metal nanopatterns or nanorods of a variety of aspect ratios. The nanopatterns fabricated from diatom have the potential of the metal-enhanced fluorescence to detect dye-conjugated molecules.
Another approach presents a platform integrating biogenic silica nanostructures with micromachined silicon substrates in a micro
ano hybrid device. In this study, one can take advantages of the unique properties of a marine diatom that exhibits nanopores on the order of 40 nm in diameter and a hierarchical structure. This device can be used to several applications, such as nano particles separation and detection. This platform is also a good substrate to study cell growth that one can observe the reaction of cell growing on the nanostructure of frustule.
ContributorsLin, Kai-Chun (Author) / Ramakrishna, B.L. (Thesis advisor) / Goryll, Michael (Thesis advisor) / Dey, Sandwip (Committee member) / Prasad, Shalini (Committee member) / Arizona State University (Publisher)
Created2014
Description
ABSTRACT The behavior of the fission products, as they are released from fission events during nuclear reaction, plays an important role in nuclear fuel performance. Fission product release can occur through grain boundary (GB) at low burnups; therefore, this study simulates the mass transport of fission gases in a 2-D GB network to look into the effects of GB characteristics on this phenomenon, with emphasis on conditions that can lead to percolation. A finite element model was created based on the microstructure of a depleted UO2 sample characterized by Electron Backscattering Diffraction (EBSD). The GBs were categorized into high (D2), low (D1) and bulk diffusivity (Dbulk) based on their misorientation angles and Coincident Site Lattice (CSL) types. The simulation was run using different diffusivity ratios (D2/Dbulk) ranging from 1 to 10^8. The model was set up in three ways: constant temperature case, temperature gradient effects and window methods that mimic the environments in a Light Water Reactor (LWR). In general, the formation of percolation paths was observed at a ratio higher than 10^4 in the measured GB network, which had a 68% fraction of high diffusivity GBs. The presence of temperature gradient created an uneven concentration distribution and decreased the overall mass flux. Finally, radial temperature and fission gas concentration profiles were obtained for a fuel pellet in operation using an approximate 1-D model. The 100 µm long microstructurally explicit model was used to simulate, to the scale of a real UO2 pellet, the mass transport at different radial positions, with boundary conditions obtained from the profiles. Stronger percolation effects were observed at the intermediate and periphery position of the pellet. The results also showed that highest mass flux happens at the edge of a pellet at steady state to accommodate for the sharp concentration drop.
ContributorsLim, Harn Chyi (Author) / Peralta, Pedro (Thesis advisor) / Dey, Sandwip (Committee member) / Sieradzki, Karl (Committee member) / Arizona State University (Publisher)
Created2011
Description
The behavior of a solid oxide fuel cell (SOFC) cermet (ceramic-metal composite) anode under reaction conditions depends significantly on the structure, morphology and atomic scale interactions between the metal and the ceramic components. In situ environmental transmission electron microscope (ETEM) is an important tool which not only allows us to perform the basic nanoscale characterization of the anode materials, but also to observe in real-time, the dynamic changes in the anode material under near-reaction conditions. The earlier part of this dissertation is focused on the synthesis and characterization of Pr- and Gd-doped cerium oxide anode materials. A novel spray drying set-up was designed and constructed for preparing nanoparticles of these mixed-oxides and nickel oxide for anode fabrication. X-ray powder diffraction was used to investigate the crystal structure and lattice parameters of the synthesized materials. Particle size distribution, morphology and chemical composition were investigated using transmission electron microscope (TEM). The nanoparticles were found to possess pit-like defects of average size 2 nm after subjecting the spray-dried material to heat treatment at 700 °C for 2 h in air. A novel electron energy-loss spectroscopy (EELS) quantification technique for determining the Pr and Gd concentrations in the mixed oxides was developed. Nano-scale compositional heterogeneity was observed in these materials. The later part of the dissertation focuses mainly on in situ investigations of the anode materials under a H2 environment in the ETEM. Nano-scale changes in the stand-alone ceramic components of the cermet anode were first investigated. Particle size and composition of the individual nanoparticles of Pr-doped ceria (PDC) were found to affect their reducibility in H2 gas. Upon reduction, amorphization of the nanoparticles was observed and was linked to the presence of pit-like defects in the spray-dried material. Investigation of metal-ceramic interactions in the Ni-loaded PDC nanoparticles indicated a localized reduction of Ce in the vicinity of the Ni/PDC interface at 420 °C. Formation of a reduction zone around the interface was attributed to H spillover which was observed directly in the ETEM. Preliminary results on the fabrication of model SOFCs and in situ behavior of Ni/Gd-doped ceria anodes have been presented.
ContributorsSharma, Vaneet (Author) / Crozier, Peter A. (Thesis advisor) / Sharma, Renu (Thesis advisor) / Adams, James B (Committee member) / Dey, Sandwip (Committee member) / Arizona State University (Publisher)
Created2011
ContributorsBrahms, Johannes, 1833-1897 (Composer)
ContributorsBrahms, Johannes, 1833-1897 (Composer)
ContributorsBrahms, Johannes, 1833-1897 (Composer)
ContributorsBrahms, Johannes, 1833-1897 (Composer)
Description
ABSTRACT
Autonomous smart windows may be integrated with a stack of active components, such as electrochromic devices, to modulate the opacity/transparency by an applied voltage. Here, we describe the processing and performance of two classes of visibly-transparent photovoltaic materials, namely inorganic (ZnO thin film) and fully organic (PCDTBT:PC70BM), for integration with electrochromic stacks.
Sputtered ZnO (2% Mn) films on ITO, with transparency in the visible range, were used to fabricate metal-semiconductor (MS), metal-insulator-semiconductor (MIS), and p-i-n heterojunction devices, and their photovoltaic conversion under ultraviolet (UV) illumination was evaluated with and without oxygen plasma-treated surface electrodes (Au, Ag, Al, and Ti/Ag). The MS Schottky parameters were fitted against the generalized Bardeen model to obtain the density of interface states (Dit ≈ 8.0×1011 eV−1cm−2) and neutral level (Eo ≈ -5.2 eV). These devices exhibited photoconductive behavior at λ = 365 nm, and low-noise Ag-ZnO detectors exhibited responsivity (R) and photoconductive gain (G) of 1.93×10−4 A/W and 6.57×10−4, respectively. Confirmed via matched-pair analysis, post-metallization, oxygen plasma treatment of Ag and Ti/Ag electrodes resulted in increased Schottky barrier heights, which maximized with a 2 nm SiO2 electron blocking layer (EBL), coupled with the suppression of recombination at the metal/semiconductor interface and blocking of majority carriers. For interdigitated devices under monochromatic UV-C illumination, the open-circuit voltage (Voc) was 1.2 V and short circuit current density (Jsc), due to minority carrier tunneling, was 0.68 mA/cm2.
A fully organic bulk heterojunction photovoltaic device, composed of poly[N-9’-heptadecanyl-2,7-carbazole-alt-5,5-(4’,7’-di-2-thienyli2’,1’,3’-benzothiadiazole)]:phenyl-C71-butyric-acidmethyl (PCDTBT:PC70BM), with corresponding electron and hole transport layers, i.e., LiF with Al contact and conducting
on-conducting (nc) PEDOT:PSS (with ITO/PET or Ag nanowire/PDMS contacts; the illuminating side), respectively, was developed. The PCDTBT/PC70BM/PEDOT:PSS(nc)/ITO/PET stack exhibited the highest performance: power conversion efficiency (PCE) ≈ 3%, Voc = 0.9V, and Jsc ≈ 10-15 mA/cm2. These stacks exhibited high visible range transparency, and provided the requisite power for a switchable electrochromic stack having an inkjet-printed, optically-active layer of tungsten trioxide (WO3), peroxo-tungstic acid dihydrate, and titania (TiO2) nano-particle-based blend. The electrochromic stacks (i.e., PET/ITO/LiClO4/WO3 on ITO/PET and Ag nanowire/PDMS substrates) exhibited optical switching under external bias from the PV stack (or an electrical outlet), with 7 s coloration time, 8 s bleaching time, and 0.36-0.75 optical modulation at λ = 525 nm. The devices were paired using an Internet of Things controller that enabled wireless switching.
Autonomous smart windows may be integrated with a stack of active components, such as electrochromic devices, to modulate the opacity/transparency by an applied voltage. Here, we describe the processing and performance of two classes of visibly-transparent photovoltaic materials, namely inorganic (ZnO thin film) and fully organic (PCDTBT:PC70BM), for integration with electrochromic stacks.
Sputtered ZnO (2% Mn) films on ITO, with transparency in the visible range, were used to fabricate metal-semiconductor (MS), metal-insulator-semiconductor (MIS), and p-i-n heterojunction devices, and their photovoltaic conversion under ultraviolet (UV) illumination was evaluated with and without oxygen plasma-treated surface electrodes (Au, Ag, Al, and Ti/Ag). The MS Schottky parameters were fitted against the generalized Bardeen model to obtain the density of interface states (Dit ≈ 8.0×1011 eV−1cm−2) and neutral level (Eo ≈ -5.2 eV). These devices exhibited photoconductive behavior at λ = 365 nm, and low-noise Ag-ZnO detectors exhibited responsivity (R) and photoconductive gain (G) of 1.93×10−4 A/W and 6.57×10−4, respectively. Confirmed via matched-pair analysis, post-metallization, oxygen plasma treatment of Ag and Ti/Ag electrodes resulted in increased Schottky barrier heights, which maximized with a 2 nm SiO2 electron blocking layer (EBL), coupled with the suppression of recombination at the metal/semiconductor interface and blocking of majority carriers. For interdigitated devices under monochromatic UV-C illumination, the open-circuit voltage (Voc) was 1.2 V and short circuit current density (Jsc), due to minority carrier tunneling, was 0.68 mA/cm2.
A fully organic bulk heterojunction photovoltaic device, composed of poly[N-9’-heptadecanyl-2,7-carbazole-alt-5,5-(4’,7’-di-2-thienyli2’,1’,3’-benzothiadiazole)]:phenyl-C71-butyric-acidmethyl (PCDTBT:PC70BM), with corresponding electron and hole transport layers, i.e., LiF with Al contact and conducting
on-conducting (nc) PEDOT:PSS (with ITO/PET or Ag nanowire/PDMS contacts; the illuminating side), respectively, was developed. The PCDTBT/PC70BM/PEDOT:PSS(nc)/ITO/PET stack exhibited the highest performance: power conversion efficiency (PCE) ≈ 3%, Voc = 0.9V, and Jsc ≈ 10-15 mA/cm2. These stacks exhibited high visible range transparency, and provided the requisite power for a switchable electrochromic stack having an inkjet-printed, optically-active layer of tungsten trioxide (WO3), peroxo-tungstic acid dihydrate, and titania (TiO2) nano-particle-based blend. The electrochromic stacks (i.e., PET/ITO/LiClO4/WO3 on ITO/PET and Ag nanowire/PDMS substrates) exhibited optical switching under external bias from the PV stack (or an electrical outlet), with 7 s coloration time, 8 s bleaching time, and 0.36-0.75 optical modulation at λ = 525 nm. The devices were paired using an Internet of Things controller that enabled wireless switching.
ContributorsAzhar, Ebraheem (Author) / Yu, Hongbin (Thesis advisor) / Dey, Sandwip (Thesis advisor) / Goryll, Michael (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2018
Description
A piezoelectric transducer, comprised of electroded and active pad PZT layer atop a backing PZT layer and protected with an acoustic matching layer, and operating under a pulse-echo technique for longitudinal ultrasonic imaging, acts as both source and detector.
Ultrasonic transducer stacks (modules), which had failed or passed during pulse-echo sensitivity testing, were received from Consortium X. With limited background information on these stacks, the central theme was to determine the origin(s) of failure via the use of thermal and physicochemical characterization techniques.
The optical and scanning electron microscopy revealed that contact electrode layers are discontinuous in all samples, while delaminations between electrodes and pad layer were observed in failed samples. The X-ray diffraction data on the pad PZT revealed an overall c/a ratio of 1.022 ratio and morphotropic boundary composition, with significant variations of the Zr to Ti ratio within a sample and between samples. Electron probe microanalysis confirmed that the overall Zr to Ti ratio of the pad PZT was 52/48, and higher amounts of excess PbO in failed samples, whereas, inductively coupled plasma mass spectrometry revealed the presence of Mn, Al, and Sb (dopants) and presence of Cu (sintering aid) in in this hard (pad) PZT. Additionally, three exothermic peaks during thermal analysis was indicative of incomplete calcination of pad PZT. Moreover, transmission electron microscopy and scanning transmission electron microscopy revealed the presence of parylene at the Ag-pad PZT interface and within the pores of pad PZT (in failed samples subjected to electric fields). This further dilutes the electrical, mechanical, and electromechanical properties of the pad PZT, which in turn detrimentally influences the pulse echo sensitivity.
Ultrasonic transducer stacks (modules), which had failed or passed during pulse-echo sensitivity testing, were received from Consortium X. With limited background information on these stacks, the central theme was to determine the origin(s) of failure via the use of thermal and physicochemical characterization techniques.
The optical and scanning electron microscopy revealed that contact electrode layers are discontinuous in all samples, while delaminations between electrodes and pad layer were observed in failed samples. The X-ray diffraction data on the pad PZT revealed an overall c/a ratio of 1.022 ratio and morphotropic boundary composition, with significant variations of the Zr to Ti ratio within a sample and between samples. Electron probe microanalysis confirmed that the overall Zr to Ti ratio of the pad PZT was 52/48, and higher amounts of excess PbO in failed samples, whereas, inductively coupled plasma mass spectrometry revealed the presence of Mn, Al, and Sb (dopants) and presence of Cu (sintering aid) in in this hard (pad) PZT. Additionally, three exothermic peaks during thermal analysis was indicative of incomplete calcination of pad PZT. Moreover, transmission electron microscopy and scanning transmission electron microscopy revealed the presence of parylene at the Ag-pad PZT interface and within the pores of pad PZT (in failed samples subjected to electric fields). This further dilutes the electrical, mechanical, and electromechanical properties of the pad PZT, which in turn detrimentally influences the pulse echo sensitivity.
ContributorsPeri, Prudhvi Ram (Author) / Dey, Sandwip (Thesis advisor) / Smith, David (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2018