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Photoelectrochemical and photophysic...
~
Zhang, Hanyu.
Photoelectrochemical and photophysical studies of carbon nanotube and molybdenum disulfide based light harvesting devices.
紀錄類型:
書目-語言資料,手稿 : Monograph/item
正題名/作者:
Photoelectrochemical and photophysical studies of carbon nanotube and molybdenum disulfide based light harvesting devices./
作者:
Zhang, Hanyu.
面頁冊數:
1 online resource (135 pages)
附註:
Source: Dissertation Abstracts International, Volume: 78-07(E), Section: B.
Contained By:
Dissertation Abstracts International78-07B(E).
標題:
Mechanical engineering. -
電子資源:
click for full text (PQDT)
ISBN:
9781369640854
Photoelectrochemical and photophysical studies of carbon nanotube and molybdenum disulfide based light harvesting devices.
Zhang, Hanyu.
Photoelectrochemical and photophysical studies of carbon nanotube and molybdenum disulfide based light harvesting devices.
- 1 online resource (135 pages)
Source: Dissertation Abstracts International, Volume: 78-07(E), Section: B.
Thesis (Ph.D.)
Includes bibliographical references
There is a critical need in utilizing solar radiation as a renewable energy source. While photovoltaic solar cells are widely used, much attention has been devoted in the past decade to developing nanotechnology for potential cost reduction and improved device efficiency and reliability. Low-dimensional materials offer unique physical properties which may be exploited for solar energy harvesting and conversion. Understanding their fundamental properties and developing relevant manufacturing strategies will thus pave the road toward high-performance, cost-effective, light-harvesting devices.
Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2018
Mode of access: World Wide Web
ISBN: 9781369640854Subjects--Topical Terms:
557493
Mechanical engineering.
Index Terms--Genre/Form:
554714
Electronic books.
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Source: Dissertation Abstracts International, Volume: 78-07(E), Section: B.
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There is a critical need in utilizing solar radiation as a renewable energy source. While photovoltaic solar cells are widely used, much attention has been devoted in the past decade to developing nanotechnology for potential cost reduction and improved device efficiency and reliability. Low-dimensional materials offer unique physical properties which may be exploited for solar energy harvesting and conversion. Understanding their fundamental properties and developing relevant manufacturing strategies will thus pave the road toward high-performance, cost-effective, light-harvesting devices.
520
$a
This thesis has investigated single-wall carbon nanotubes (SWCNTs) and molybdenum disulfide (MoS2) nanolayers for their light-harvesting ability in donor-acceptor systems. These materials were studied with three specific goals: (i) introducing innovative light-harvesting designs, (ii) understanding their fundamental photophysical and photoelectrochemical properties, and (iii) providing potential solutions to improve the system performance.
520
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First, novel light-harvesting complexes were designed using semiconducting SWCNTs and cationic porphyrins as acceptors and donors, respectively. These complexes were assembled by synthetic DNA oligonucleotides that recognize porphyrins, while noncovalently functionalizing SWCNTs. The SWCNT-DNA-porphyrin hybrids were used to manufacture large-area thin films through solution-phase processing and membrane filtration methods. From extensive studies of optical absorption, emission, and photocurrents, new detailed insights on photo-processes were gained for photoelectrochemical conversion.
520
$a
A regenerative donor-acceptor light-harvesting system was introduced and demonstrated to counteract photoinduced degradation of porphyrin molecules. The photo-damaged chromophores were dissociated from the complex by modulating the chemical environment, while DNA-SWCNTs were preserved. When fresh porphyrins were reintroduced and reassociated with DNA-SWCNTs, photocurrents were fully recovered. As proof-of-principle, A 50% increase in photocurrents was demonstrated through four successive regenerations within 90 minutes, compared to the complex without regeneration. Such dynamic strategy could improve the overall device efficiency and extend the operation lifetime.
520
$a
Lastly, a novel solution-phase manufacturing process was developed to fabricate large-area two-dimensional MoS2 nanolayers for light harvesting applications. The MoS2 nanolayers were functionalized with 8 porphyrin species from 3 families to mitigate charge recombination by defects and small crystallites. A strong correlation between porphyrin species and photocurrents was observed, where interfacial porphyrins suppress charge recombination within MoS2 nanolayers, thus enhancing the photoelectrochemical performance of the devices. A photocurrent enhancement mechanism was proposed based on the energy difference between the valence band of MoS2 and highest occupied molecular orbital level of porphyrins.
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Overall, the innovative designs and the scientific insights on photophysics and photoelectrochemical conversion in this thesis will form the basis for developing next-generation solar energy harvesting devices.
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