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.

利用太阳能将二氧化碳和水转化为有用的化学品和燃料可以提供可持续碳循环的途径，同时维持化学和运输行业的现有基础设施。有效利用太阳能来打破稳定的二氧化碳键是该过程的第一步，并且需要调整用于该反应的催化剂的光物理性质。在这个项目中，教授。俄亥俄州立大学的古普塔和阿斯哈吉里正在努力了解催化剂表面结构与太阳能转移到二氧化碳分子之间的关系。目标是了解促进这种能量转移和促进二氧化碳转化的因素。作为该项目的一部分，PI 正在培训研究生将实验和理论结合起来，解决重要的能源产生和转换问题。此外，PI 还吸引了 K-12 和本科生的学生，作为扩大学生参与 STEM 职业的多元化努力的一部分。作为俄亥俄州立大学 TEK8 计划的一部分，研究生正在开发模块，以吸引 K-12 学生对 STEM 职业的兴趣。此外，作为俄亥俄州立大学夏季研究机会计划的一部分，还招募了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，俄亥俄州立大学的 Gupta 博士和 Asthagiri 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局部表面结构与铜氧化物之间的关系。 CO2 分子的光激发。氧化铜薄膜在超高真空 (UHV) 中以受控方式生长，允许引入各种缺陷（例如空位、氧化铜薄膜化学计量的变化和掺杂剂）。具有局部光照明功能的扫描隧道显微镜 (STM) 可提供照明前后表面的直接图像。密度泛函理论 (DFT) 计算有助于解释 STM 的图像和光谱，以将局部氧化铜位点的电子态与由此产生的 CO2 光化学之间的关系联系起来。此外，DFT 还被用来探索对 Cu 氧化膜的修饰，以增强 CO2 光活化；这些预测正在进行实验测试，目的是建立用于 CO2 光还原的最佳氧化铜纳米结构的预测模型。作为该项目的一部分，PI 积极参与招募研究生和本科生研究和开发模块中代表性不足的群体，以通过俄亥俄州立大学的 TEK8 计划培养 K-12 学生对 STEM 职业的兴趣。该奖项反映了 NSF 的法定使命和通过使用基金会的智力优点和更广泛的影响审查标准进行评估，该项目被认为值得支持。

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