Energy funneling in plasmonic nanocrystal composites for photocatalytic production of solar fuels

用于光催化生产太阳能燃料的等离子体纳米晶体复合材料中的能量漏斗

• 批准号: 1465052
• 负责人: Mikhail Zamkov
• 金额: $ 37.4万
• 依托单位: Bowling Green State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-09-01 至 2019-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1465052&HistoricalAwards=false
• 关键词: Energy; funneling; plasmonic; nanocrystal; composites

Energy funneling in plasmonic nanocrystal composites for photocatalytic production of solar fuels.Dr. Mikhail Zamkov of Bowling Green State University is developing a novel model system for solar energy conversion in colloidal nanostructures aimed toward improving their photocatalytic activity. The proposed nanomaterial architecture is designed to funnel the solar light into the center of a composite nanoparticle via a built-in antenna. The absorbed radiation is then routed toward the exterior of the nanoparticle to drive catalytic reactions on its surface. To enable an efficient catalytic cycle, a novel type of energy transfer mechanism between the antenna and the catalyst is employed. The proposed innovation makes use of judiciously engineered interfaces between inorganic domains of the composite nano-object to ensure a seamless transfer of the solar energy across the photocatalytic system. The catalytic nanostructures are rendered soluble, which allows combing the benefits of homogenous reactions on the surface (excellent activity and selectivity) with the facility of the heterogeneous systems to recycle the catalyst. These materials are particularly suited to drive aqueous phase reactions, including hydrogen production and environmental clean-up, with enhanced reactivity under the solar flux. The proposed project helps the investigator in his effort to continue to bring in several students from underrepresented groups each summer for a full-time research internship in the lab. The investigator also interfaces with several industrial partners to provide the undergraduate researchers with industrial laboratory experience.In this project, funded by the Chemical Catalysis Program, Dr. Mikhail Zamkov of Bowling Green State University focuses on the synergy of novel synthetic strategies and ultrafast spectroscopy techniques to explore a new class of photocatalytic materials utilizing composite colloidal nanostructures. The proposed nanomaterials combine several inorganic domains in a single nano-reactor designed to efficiently convert the solar radiation into a catalytically active state. The key innovation of the nanomaterial architecture lies in the plasmon-assisted light-harvesting scheme, which takes advantage of the strong electro-magnetic field that exists in metal nanoparticles to boost the production of excitons in the surrounding semiconductor shell. The excitation energy of the shell is then relayed to suitable oxidation/reduction catalysts on the surface. To ensure that different constituents of the composite nano-object work seamlessly, inter-domain interfaces are grown using molecular epitaxy. Such stoichiometric bonds, either covalent or ionic, reduce the density of defect states that dissipate the excitation energy enabling a high throughput of the absorbed radiation. The catalytic performance of the investigator's colloidal nanostructures are tested using common redox reactions in aqueous media, while the energy transfer processes are investigated using ultrafast spectroscopy techniques. As an active member of Building Ohio's Sustainable Energy Future and Science, Engineering & Technology Gateway Ohio programs, Professor Zamkov involves small teams of undergraduate students in this research project, introducing them to general concepts in ultrafast spectroscopy, material science, and chemical synthesis. Special efforts are made to involve minority students and students from underrepresented groups. Professor Zamkov also interfaces with several industrial partners to provide the undergraduate researchers with industrial laboratory experience.

等离激元纳米晶体复合材料的能量漏斗，用于光催化的太阳能燃料。鲍灵格林州立大学的Mikhail Zamkov正在开发一种新型模型系统，用于胶体纳米结构中的太阳能转化，旨在改善其光催化活性。拟议的纳米材料结构旨在通过内置天线将太阳能光融入复合纳米颗粒的中心。然后将吸收的辐射路由朝向纳米颗粒的外部，以驱动其表面催化反应。为了实现有效的催化循环，采用了天线和催化剂之间的新型能量转移机制。提出的创新利用了复合纳米对象的无机域之间的明智设计的界面，以确保太阳能在光催化系统中无缝传递。催化纳米结构是可溶性的，它允许将表面上均匀反应的益处（优秀的活性和选择性）与异质系统的设施梳理，以回收催化剂。这些材料特别适合推动水相反应，包括氢的产生和环境清理，在太阳通量下具有增强的反应性。拟议的项目可以帮助调查人员每年夏天继续吸引来自代表性不足小组的几名学生在实验室中进行全日制研究实习。研究人员还与几个工业伙伴交织在一起，以向本科研究人员提供工业实验室的经验。在该项目中，由化学静脉毒性计划资助，鲍林绿色州立大学的Mikhail Zamkov博士重点介绍了新型的Synthetic策略和超级型光谱技术的协同作用，以探索一种新型的光电材料综合材料，以探索新型的综合材料。提出的纳米材料在单个纳米反应器中组合了几个无机域，旨在有效地将太阳辐射转化为催化活性状态。纳米材料结构的关键创新在于等离子辅助的轻度收获方案，该方案利用了在金属纳米颗粒中存在的强烈电磁场，以增强周围半管壳中激子的产生。然后将壳的激发能中继到表面上合适的氧化/还原催化剂。 为了确保复合纳米对象的不同成分无缝地工作，使用分子外延生长域间界面。这种化学计量键是共价或离子的，它降低了耗散激发能量的缺陷密度，从而使吸收的辐射的高通量能够散发出。研究者的胶体纳米结构的催化性能使用水性介质中的常见氧化还原反应进行了测试，同时使用超快光谱技术研究了能量传递过程。 作为俄亥俄州建筑可持续能源和科学，工程与技术网关计划的积极成员，Zamkov教授涉及本研究项目的小型本科生团队，将其介绍给超级光谱，材料科学和化学合成中的一般概念。做出了特别的努力，以涉及少数族裔学生和代表性不足的团体的学生。 Zamkov教授还与几个工业合作伙伴互动，为本科研究人员提供工业实验室的经验。

项目成果

Just Add Ligands: Self-Sustained Size Focusing of Colloidal Semiconductor Nanocrystals

只需添加配体：胶体半导体纳米晶体的自我维持尺寸聚焦

• DOI: 10.1021/acs.chemmater.7b05165
• 发表时间: 2018
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Razgoniaeva, Natalia;Yang, Mingrui;Garrett, Paul;Kholmicheva, Natalia;Moroz, Pavel;Eckard, Holly;Royo Romero, Luis;Porotnikov, Dmitry;Khon, Dmitriy;Zamkov, Mikhail
• 通讯作者: Zamkov, Mikhail