Surface science studies of the photo physics of copper oxides: toward sustainable CO2 recycling

氧化铜光物理的表面科学研究：实现可持续的二氧化碳回收

• 批准号: 1809837
• 负责人: Jay Gupta
• 金额: $ 46.5万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1809837&HistoricalAwards=false
• 关键词: Surface; science; studies; photo; physics

Solar conversion of CO2 and water to useful chemicals and fuels can provide a pathway to a sustainable carbon cycle, while maintaining existing infrastructure in the chemical and transport industries. Efficient use of solar energy to break the stable CO2 bonds is the first step in this process and requires tailoring the photophysical properties of the catalysts used for that reaction. In this project, Profs. Gupta and Asthagiri of Ohio State University are working to understand the relationship between catalyst surface structure and solar energy transfer into the CO2 molecule. The goal is to understand the factors that promote this energy transfer and promote CO2 conversion. As part of this project, the PIs are training graduate students to combine experiment and theory to tackle important energy generation and conversion problems. In addition, the PIs are engaging students from the K-12 and undergraduate level as part of an outreach effort to diversify student participation in STEM careers. Graduate students, as part of Ohio State's TEK8 program, are developing modules to engage K-12 students interest in STEM careers. In addition, underrepresented undergraduate students are being recruited for summer research as part of Ohio State's Summer Research Opportunities Program. With funding from the NSF Chemical Catalysis program of the Chemistry Division, Dr. Gupta and Asthagiri from The Ohio State University are developing a program that combines experiment and theory aimed to gain a fundamental understanding of the relationship between local surface structure of Cu oxides and the photoexcitation of CO2 molecules. Cu oxide thin films are grown in a controlled fashion in ultrahigh vacuum (UHV) that allows for the introduction of various defects (e.g. vacancies, variation in Cu oxide film stoichiometry, and dopants). Scanning tunneling microscopy (STM) with local photoillumination provide direct images of the surface before and after illumination. Density functional theory (DFT) calculations are assisting in interpreting both the images and spectroscopy from STM to link the relationship between the electronic states of the local Cu oxide site and the resulting CO2 photochemistry. In addition, DFT is being used to explore modifications to the Cu oxide films that enhance CO2 photoactivation; these predictions are being tested experimentally with the goal to establish a predictive model for optimal Cu oxide nanostructures for CO2 photoreduction. As part of this project, the PIs are actively engaged in the recruitment of underrepresented groups in graduate and undergraduate research and developing modules to foster the interest in STEM careers of K-12 students through Ohio State's TEK8 program.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

太阳能将二氧化碳和水转化为有用的化学品和燃料，可以为可持续的碳循环提供一条途径，同时维护化学和运输行业的现有基础设施。有效利用太阳能来破坏稳定的CO2键是该过程的第一步，需要定制用于该反应的催化剂的物理化学性质。在这个项目中，教授。俄亥俄州州立大学的古普塔和阿斯塔吉里正在研究催化剂表面结构与太阳能转化为二氧化碳分子之间的关系。我们的目标是了解促进这种能量转移和促进CO2转化的因素。作为该项目的一部分，PI正在培训研究生将联合收割机实验和理论结合起来，以解决重要的能源生产和转换问题。此外，PI正在吸引K-12和本科生的学生，作为外展工作的一部分，以使学生参与STEM职业。研究生，作为俄亥俄州的TEK 8计划的一部分，正在开发模块，以吸引K-12学生对STEM职业的兴趣。此外，作为俄亥俄州夏季研究机会计划的一部分，正在招募代表性不足的本科生进行夏季研究。在美国国家科学基金会化学部化学催化项目的资助下，来自俄亥俄州州立大学的Gupta博士和Asthagiri博士正在开发一个结合实验和理论的项目，旨在从根本上了解铜氧化物的局部表面结构与CO2分子的光激发之间的关系。铜氧化物薄膜生长在可控的方式在超真空（UHV），允许引入各种缺陷（如空位，铜氧化物膜化学计量的变化，和掺杂剂）。具有局部光照明的扫描隧道显微镜（STM）提供照明之前和之后的表面的直接图像。密度泛函理论（DFT）计算有助于解释STM的图像和光谱，以将局部Cu氧化物位点的电子态与所产生的CO2光化学之间的关系联系起来。此外，DFT被用来探索修改的铜氧化物薄膜，提高二氧化碳的光活化，这些预测正在进行实验测试，目标是建立一个预测模型的最佳铜氧化物纳米结构的二氧化碳光还原。作为该项目的一部分，PI积极参与研究生和本科生研究和开发模块中代表性不足的群体的招聘，以通过俄亥俄州的TEK 8计划培养K-12学生对STEM职业的兴趣。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估来支持。

项目成果

Tunable tunnel barriers in a semiconductor via ionization of individual atoms

通过单个原子的电离可调节半导体中的隧道势垒

• DOI: 10.1088/1361-648x/abf9bd
• 发表时间: 2021
• 期刊: Journal of Physics: Condensed Matter
• 作者: Mueller, Sara M;Kim, Dongjoon;McMillan, Stephen R;Tjung, Steven J;Repicky, Jacob J;Gant, Stephen;Lang, Evan;Bergmann, Fedor;Werner, Kevin;Chowdhury, Enam
• 通讯作者: Chowdhury, Enam