CAREER: Elucidating the Interfacial Structure of Complex Solvents for Chemical Transformations

职业：阐明化学转化复杂溶剂的界面结构

• 批准号: 2045111
• 负责人: Burcu Gurkan
• 金额: $ 55万
• 依托单位: Case Western Reserve University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2026-08-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2045111&HistoricalAwards=false
• 关键词: CAREER; Elucidating; Interfacial; Structure; Complex

The availability of high-performing solvents that function as absorbents, co-catalysts, and electrolytes is a critical and unmet need for advanced technologies such as integrated capture and conversion of carbon dioxide. This project will develop functionalized solvents that have high affinity to carbon dioxide as well as facilitate its efficient conversion to other useful products such as fuels. These complex solvents are hydrogen-bonded organic complex (HBOC) liquids with high concentrations of salts and often have molecular-scale structure and heterogeneity. The mechanisms of absorption and reactivity of carbon dioxide at the electrode-electrolyte interface are not well understood in these solvents. This project will explore the fundamental mechanisms that underpin absorption, interfacial liquid structure, and reactivity to inform future designs of integrated systems for chemical transformations. The knowledge gained has far-reaching applications in separations, catalysis, sensors, and other electrochemical processes. Through these applications, this research addresses the societal challenges of climate change, emission mitigation, waste utilization, and energy consumption. The educational goal of this CAREER project is to enhance students’ learning experience using visuals and to build science literacy through drawing. Visual illustrations of the scientific concepts of this project will be created for use as educational materials, which will be disseminated via publications, seminars, and public events. These activities will foster teamwork and strengthen ties with the local community in Cleveland through collaboration with the Cleveland Institute of Art.With support from both the Interfacial Engineering and Electrochemical Systems programs, this project will characterize the liquid structure of concentrated electrolytes at interfaces with electrified surfaces and quantitatively assess the structural impact on charge distribution, thermodynamics, and reaction mechanisms in separation processes and electrochemical reactions. The solvation structure and reactive state of the carbon dioxide model compound both within and at HBOC electrolyte-electrode interfaces will be investigated by spectroscopy, neutron and X-ray reflectivity, and electroanalytical techniques. These studies will provide a basis for understanding the structure and dynamics of the behavior of small molecules in complex solvents. More specifically, the following scientific questions will be answered: (1) What is the physical environment of the carbon dioxide solvate complex at the electrode-electrolyte interface? and (2) What is the impact of the interface structure on electron and proton transfer and selectivity of the carbon dioxide reduction mechanism? The results from this study will contribute to the understanding of electrical double layer structures of HBOC electrolytes, as they cannot be explained by the traditional models suitable for dilute systems. The results will also impact the discussions on the role of the electrolyte in carbon dioxide co-catalysis. The project will apply the STEM educational concept of ‘learning by drawing’ and artistic illustration in undergraduate and graduate-level courses and public outreach. Learning by drawing is expected to enhance student engagement in engineering courses, improve visual literacy, promote knowledge retention, increase diversity among students pursuing STEM-related fields, as well foster interdisciplinary communication between art and engineering students.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.

对吸收剂，共催化剂和电解质的高性能解决方案的可用性是对先进技术的关键且未满足的需求，例如综合捕获和二氧化碳的转化。该项目将开发功能化的解决方案，这些解决方案对二氧化碳具有高亲和力，并促进其有效转化为其他有用产品（例如燃料）。这些复合溶液是氢键有机络合物（HBOC）液体，具有高浓度的盐，通常具有分子规结构和异质性。在这些溶液中，二氧化碳在电极 - 电解质界面上的分析和反应性机制尚不很好。该项目将探讨滥用滥用，界面液体结构和反应性的基本机制，以告知对化学转化集成系统的未来设计。获得的知识在分离，催化，传感器和其他电化学过程中具有深远的应用。通过这些应用，这项研究解决了气候变化，缓解排放，废物利用和能源消耗的社会挑战。这个职业项目的教育目标是使用视觉效果增强学生的学习经验，并通过绘画来建立科学素养。将创建有关该项目科学概念的视觉插图，以用作教育材料，该材料将通过出版物，半手和公共事件进行传播。这些活动将通过与克利夫兰艺术学院的合作来促进团队合作，并加强与克利夫兰的当地社区的联系。与界面工程和电化学系统计划的支持，该项目将在电动表面界面上集中电解质的液体结构与电力表面的液体结构进行表征，并对电荷分离和反应的结构进行分离，并分离型和热反应和反应，并分离出对电型和反应的反应，并具有分离的效果。二氧化碳模型的溶液结构和反应性态在HBOC电解质电极界面内外都将通过光谱，中子和X射线反射率以及电分析技术研究。这些研究将为理解复杂求解器中小分子行为的结构和动力学提供基础。更具体地说，将回答以下科学问题：（1）在电极 - 电解质界面上解决了二氧化碳的物理环境是什么？ （2）界面结构对电子和质子转移以及二氧化碳还原机制的选择性有什么影响？这项研究的结果将有助于理解HBOC电解质的电气双层结构，因为它们无法通过适合稀释系统的传统模型来解释。结果还将影响有关电解质在二氧化碳共催化中的作用的讨论。该项目将在本科和研究生级课程以及公共宣传中应用“通过绘画和艺术插图学习”和“学习”的STEM教育概念。预计通过绘画学习将增强学生参与工程课程，提高视觉素养，促进知识保留，增加追求与STEM相关领域的学生之间的多样性，以及促进艺术与工程学生之间的跨学科沟通。该奖项反映了NSF的法定任务，并通过该基金会的知识优点和广泛的影响来评估NSF的法定任务。