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| Collaborative Proposal: Fire, dust, air and water: Improving aerosol biogeochemistry interactions in ACME | |
| 项目编号 | DE-SC0016321 |
| Bond, Tami | |
| 项目主持机构 | Board of Trustees of the University of Illinois |
| 开始日期 | 2016-09-01 |
| 结束日期 | 2019-08-31 |
| 英文摘要 | The use of sunlight to drive the conversion of CO2 and water to organic products provides a strategy for both mitigating dependence on fossil fuels and ameliorating the dumping of CO2 into the atmosphere. It has been demonstrated that many of the known limitations could be overcome by employing aqueous pyridinium as an electrocatalysts for the formation of methanol from CO2(aq). In this work, an illuminated p-GaP photocathode was employed in a system that produced methanol with 96% faradaic efficiency at a ~200mV underpotential. Improvement of this system requires a mechanistic understanding of the catalytic process. The experimental finding is that a strong interaction occurs between pyridine (or pyridinium) and the electrode surface. The nature of that interaction and how it leads to an electrocatalytic environment is a focus of this work. This line of reasoning suggests that interfaces can be designed that either interact with a molecular catalyst such as pyridine or CO2 itself to facilitate the reduction of interest. The similarity in redox potential for CO2 and H2O reduction and the fact that some semiconductors are specific for one reaction over the other, suggests that an understanding of these specific surface interactions is critical to further development of solar fuel forming interfaces. To this end, work will continue on single crystal p-GaP interfaces, as well as on under explored p-type semiconductors as photocathodes. Three themes will be pursued under this research proposal: 1) A continued exploration of single crystal, p-type, III-V photocathodes to identify the specific interfacial features that facilitate charge transfer to aromatic amines; 2) Exploration of p-type metal oxide delafossite phase semiconductor electrodes. This class of solids can be energetically tuned to enhance interfacial photoinduced charge transfer kinetics directly to CO2; and 3) Metal chalcopyrites of the form Cu(InxGa1-x)(Se,S)2 (CIGS) offer another type of system where band edge energies are well established. These semiconductors have been lightly explored with respect to water splitting, with even less work presented with regard to CO2 reduction. Single crystal samples of these materials offer an opportunity to probe the relationship between electrode surface composition and electrocatalytic activity for both water splitting and CO2 reduction. It is anticipated that new semiconductor materials and new aromatic amine catalyst will be developed as a result of these studies, and that the findings will advance photoelectrochemical science toward the goal of generating hydrocarbon based, liquid solar fuels under practical conditions. |
| 学科分类 | 09 - 环境科学;06 - 生物科学 |
| 资助机构 | US-DOE |
| 项目经费 | 281213.39 |
| 项目类型 | Cooperative Agreement |
| 国家 | US |
| 语种 | 英语 |
| 文献类型 | 项目 |
| 条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/73734 |
| 推荐引用方式 GB/T 7714 | Bond, Tami.Collaborative Proposal: Fire, dust, air and water: Improving aerosol biogeochemistry interactions in ACME.2016. |
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