CAREER: Rational Design of Novel Electrocatalyst with Enhanced Properties

职业：合理设计具有增强性能的新型电催化剂

• 批准号: 1350911
• 负责人: Feng Jiao
• 金额: $ 40万
• 依托单位: University of Delaware
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-07-01 至 2019-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1350911&HistoricalAwards=false
• 关键词: CAREER; Rational; Design; Novel; Electrocatalyst

Title: Rational Design of Carbon Dioxide Reduction Electrocatalysts with Enhanced PropertiesReuse of carbon dioxide emissions from fossil fuel utilization is beneficial for human society. In the past decade, researchers have extensively studied a wide range of catalysts with activity to convert carbon dioxide into useful chemicals in an efficient and selective way. Copper is the most widely used electrocatalyst for carbon dioxide reduction, because of its abundance and unique capability to produce hydrocarbons. However, two unsolved major drawbacks of copper catalysts are the poor selectivity and large overpotential. In order to address these challenges, a highly integrated approach is proposed by CAREER award winner Feng Jiao at the University of Delaware to explore bimetallic catalysts as potential candidates. The proposed program combines computational modeling, experimental assessment, and advanced characterization methods, which will greatly advance the fundamental understanding of carbon dioxide reduction on the surface of bimetallic catalysts. The knowledge generated in the proposed research will be utilized to develop efficient liquid transportation fuel production systems using renewable energy and some of the carbon dioxide emitted from various combustion sources. Additionally, the proposed program will broaden the participation of the underrepresented groups, especially African American students, and inspire the young generation to develop a long-term interest in STEM subjects.The goal of this CAREER proposal is to establish an integrated research platform for the development of novel copper-based bimetallic carbon dioxide reduction electrocatalysts with enhanced efficiency and selectivity. The proposed research program consists of three major tasks: first-principles modeling of carbon dioxide electroreduction on ideal bimetallic catalysts, experimental investigation of the kinetics on prototype bimetallic systems, and advanced in-situ structural characterization methods. A systematic study of the reactivity on various copper-based bimetallic surfaces will be performed using first-principle methods. The outcome will provide guidance for designing more active and selective bimetallic electrocatalysts. In parallel, efforts will be devoted to the synthesis of copper-based bimetallic thin films, the investigation of carbon dioxide electroreduction kinetics, and the assessment of model predictions. The combination of first-principle calculations and experimental efforts will lead to fundamental insights and development of the structure-reactivity correlation in copper-based bimetallic electrocatalysts for carbon dioxide reduction. Additionally, in-situ structural diagnostic tools will be developed through collaborations with scientists in the national laboratories. The tools will enable the monitoring of catalytic reactions at molecular level under realistic conditions in real time. The integration of these pillars will set the foundations for the long-term career in heterogeneous catalysis research for Dr. Jiao.

标题：合理设计具有增强性能的二氧化碳还原电催化剂重新利用化石燃料使用中排放的二氧化碳对人类社会有益。在过去的十年中，研究人员广泛研究了各种催化剂，这些催化剂具有以有效和选择性的方式将二氧化碳转化为有用化学品的活性。铜是最广泛使用的二氧化碳还原电催化剂，因为它储量丰富且具有独特的生产碳氢化合物的能力。然而，铜催化剂的两个尚未解决的主要缺点是选择性差和过电势大。为了应对这些挑战，特拉华大学职业奖获得者焦峰提出了一种高度集成的方法来探索双金属催化剂作为潜在的候选者。该计划结合了计算建模、实验评估和先进的表征方法，这将极大地促进对双金属催化剂表面二氧化碳还原的基本理解。拟议研究中产生的知识将用于开发高效的液体运输燃料生产系统，该系统使用可再生能源和各种燃烧源排放的一些二氧化碳。此外，该计划将扩大代表性不足的群体，特别是非裔美国学生的参与，并激发年轻一代对STEM学科的长期兴趣。该职业计划的目标是建立一个综合研究平台，用于开发新型铜基双金属二氧化碳还原电催化剂，提高效率和选择性。拟议的研究计划包括三个主要任务：理想双金属催化剂上二氧化碳电还原的第一原理建模、原型双金属系统动力学的实验研究以及先进的原位结构表征方法。将使用第一原理方法对各种铜基双金属表面的反应性进行系统研究。该结果将为设计更具活性和选择性的双金属电催化剂提供指导。与此同时，还将致力于铜基双金属薄膜的合成、二氧化碳电还原动力学的研究以及模型预测的评估。第一原理计算和实验工作的结合将带来对用于二氧化碳还原的铜基双金属电催化剂的结构-反应性相关性的基本见解和发展。此外，将通过与国家实验室的科学家合作开发现场结构诊断工具。这些工具将能够在现实条件下实时监测分子水平的催化反应。这些支柱的整合将为焦博士在多相催化研究领域的长期职业生涯奠定基础。