Photolytic Nanoconjugate Fuel Generators

光解纳米共轭燃料发生器

• 批准号: 1707008
• 负责人: Kaan Kalkan
• 金额: $ 29.97万
• 依托单位: Oklahoma State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-09-01 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1707008&HistoricalAwards=false
• 关键词: Photolytic; Nanoconjugate; Fuel; Generators

The project is focused on designing a photoelectrochemical device that can potentially be scaled up to the size of 'photolysis farms' capable of the commercial-scale production of hydrogen obtained from the photocatalytic splitting of water. The produced hydrogen (H2) could be used directly for energy generation (i.e. solar fuel) or as a feedstock for the generation of sustainable liquid fuels or chemicals. The immediate focus of the project would be on both understanding the working mechanism and optimizing the efficiency of so-called nanoconjugate devices based on semiconductor nanowires decorated with metal nanoparticles. The project will involve collaboration with a commercial partner for student training and investigation of early stage manufacturing feasibility, and will also incorporate several outreach activities on nanoparticles and microscopy for K-12 students.The research is built on the hypothesis that a combination of electronic, electrostatic, and plasmonic mechanisms can be achieved by utilizing the nanoconjugate device structure with appropriate materials. Preliminary results from the investigator's laboratory have already demonstrated 5.6% light-to-hydrogen efficiency with a H2 to O2 ratio of 2.0 under 445 nm radiation using sol-gel prepared vanadium oxyhydrate nanowires coated with nanogold. The unique architecture of the nanowire-nanoparticle device enables a novel combination of effects and mechanisms that can potentially increase photolytic efficiency. Mechanisms to be investigated are: 1) self-alignment of electron energy levels due to ultralow nanoparticle capacitance, 2) surface-charge-enabled alignment of energy levels with redox levels, and 3) direct plasmon-driven reduction by chemical interface damping. The elucidation of these enabling mechanisms should potentially impact other novel photocatalyst development efforts and allow for a larger set of photocatalytic materials and structures capable of photolysis. The project will utilize and investigate V2O5-H2O as the photoanode, which is essentially a little-known semiconductor. The system to be investigated has been chosen with scale-up in mind, as the photolytic nanoconjugates can be manufactured at low cost in the form of an aqueous suspension, which subsequently can be filled in transparent enclosure panels and scaled up to a fuel farm. To this end, the project will collaborate with InnoVital Systems, Inc. of Maryland to develop student internships. Under the direction of the InnoVital engineers, undergraduate engineering students will be engaged in designing a glass/plastic enclosure for the nanodevice suspension that will serve as an advanced prototype of the photolytic panel. Outreach activities will center on one-day summer camps carried out in collaboration with Oklahoma WONDERtorium, where the children will make nanoparticles with kits developed by the project team and examine their nanoparticles using optical and electron microscopy. Additionally, the project will engage underrepresented students in research through the Oklahoma Louis Stokes Alliance for Minority Participation Scholars Program (OK-LSAMP).

该项目的重点是设计一种光电化学设备，该设备可以扩大到“光解农场”的规模，能够从光催化分解水获得商业规模的氢气生产。 产生的氢气（H2）可以直接用于能源生产（即太阳能燃料）或作为可持续液体燃料或化学品生产的原料。 该项目的直接重点将是了解工作机制和优化基于金属纳米颗粒装饰的半导体纳米线的所谓纳米共轭器件的效率。 该项目将涉及与商业合作伙伴的学生培训和早期制造可行性的调查合作，也将包括几个外展活动的纳米粒子和显微镜的K-12 students.The研究是建立在假设的电子，静电和等离子体激元机制的组合，可以通过利用纳米共轭器件结构与适当的材料实现。 研究人员实验室的初步结果已经证明，使用溶胶-凝胶制备的涂覆有纳米金的氢氧化钒纳米线，在445 nm辐射下，H2与O2的比率为2.0，光氢效率为5.6%。 纳米颗粒装置的独特结构使得能够实现可以潜在地增加光解效率的效应和机制的新颖组合。 待研究的机制是：1）由于超低纳米颗粒电容导致的电子能级的自对准，2）表面电荷使能的能级与氧化还原能级的对准，以及3）通过化学界面阻尼的直接等离子体驱动的还原。 这些使能机制的阐明可能会影响其他新型光催化剂的开发工作，并允许更多的光催化材料和结构能够光解。 该项目将利用和研究V2 O 5-H2O作为光阳极，这基本上是一种鲜为人知的半导体。 选择要研究的系统时考虑到了放大，因为光解纳米缀合物可以以低成本以水悬浮液的形式制造，随后可以将其填充在透明的封闭面板中并放大到燃料农场。 为此，该项目将与InnoVital Systems，Inc.合作。马里兰州发展学生实习。 在InnoVital工程师的指导下，本科工程专业的学生将参与设计一个用于纳米器件悬挂的玻璃/塑料外壳，该外壳将作为光解面板的先进原型。 外展活动将集中在为期一天的夏令营与俄克拉荷马州WONDERTorium合作开展，在那里，孩子们将与项目小组开发的套件，使纳米粒子和检查他们的纳米粒子使用光学和电子显微镜。 此外，该项目将通过俄克拉荷马州路易斯·斯托克斯少数民族参与学者计划联盟（OK-LSAMP）让代表性不足的学生参与研究。

项目成果

Cuprous Oxide Cubic Particles with Strong and Tunable Mie Resonances for Use as Nanoantennas

• DOI: 10.1021/acsanm.0c01201
• 发表时间: 2020-06
• 作者: Farshid Mohammadparast;S. Ramakrishnan;Nishant Khatri;Ravi Teja A. Tirumala;Susheng Tan;A. Kalkan;M. Andiappan

Electrochemical and Surface-Plasmon Correlation of a Serum-Autoantibody Immunoassay with Binding Insights: Graphenyl Surface versus Mercapto-Monolayer Surface

• DOI: 10.1021/acs.analchem.8b01565
• 发表时间: 2018-11-06
• 期刊: ANALYTICAL CHEMISTRY
• 影响因子: 7.4
• 作者: Premaratne, Gayan;Niroula, Jinesh;Krishnan, Sadagopan
• 通讯作者: Krishnan, Sadagopan

C–C Coupling Reactions Catalyzed by Gold Nanoparticles: Evidence for Substrate-Mediated Leaching of Surface Atoms Using Localized Surface Plasmon Resonance Spectroscopy

金纳米粒子催化的 C–C 偶联反应：使用局域表面等离子共振光谱进行基质介导的表面原子浸出的证据

• DOI: 10.1021/acs.jpcc.8b12453
• 发表时间: 2019
• 期刊: The Journal of Physical Chemistry C
• 作者: Mohammadparast, Farshid;Dadgar, Andishaeh P.;Tirumala, Ravi Teja;Mohammad, Sayeed;Topal, C. Ozge;Kalkan, A. Kaan;Andiappan, Marimuthu
• 通讯作者: Andiappan, Marimuthu

Structure–Property–Performance Relationships of Cuprous Oxide Nanostructures for Dielectric Mie Resonance-Enhanced Photocatalysis

• DOI: 10.1021/acscatal.2c00977
• 发表时间: 2022-06
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Ravi Teja A. Tirumala;Sunil Gyawali;Aaron Wheeler;S. Ramakrishnan;R. Sooriyagoda;Farshid Mohammadparast;Nishant Khatri;Susheng Tan;A. Kalkan;Alan D Bristow;M. Andiappan

Cupric Oxide Mie Resonators

• DOI: 10.1021/acs.jpcc.2c04646
• 发表时间: 2022-09
• 期刊: The Journal of Physical Chemistry C
• 作者: S. Ramakrishnan;Nishant Khatri;Ravi Teja Addanki Tirumala;Farshid Mohammadparast;Krishnageetha Karuppasamy;A. Kalkan;M. Andiappan