CAREER: Rational Design of Novel Electrocatalyst with Enhanced Properties

题目：高性能二氧化碳还原电催化剂的合理设计化石燃料利用产生的二氧化碳的再利用对人类社会是有益的。在过去的十年里，研究人员广泛地研究了各种各样的催化剂，这些催化剂具有将二氧化碳高效和选择性地转化为有用的化学物质的活性。铜是最广泛使用的二氧化碳还原电催化剂，因为它的丰富和独特的能力产生碳氢化合物。但铜催化剂的两个主要缺点是选择性差和过电位大。为了应对这些挑战，特拉华大学的CAREER奖获得者Feng Jiao提出了一种高度集成的方法，探索双金属催化剂作为潜在的候选材料。该方案将计算建模、实验评估和先进的表征方法相结合，将极大地促进对双金属催化剂表面二氧化碳还原的基本认识。在拟议的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，拟议的项目将扩大代表性不足的群体，特别是非洲裔美国学生的参与，并激励年轻一代培养对STEM学科的长期兴趣。本项目旨在为新型铜基双金属二氧化碳还原电催化剂的开发提供一个综合研究平台，以提高效率和选择性。本研究主要包括三个方面：理想双金属催化剂上二氧化碳电还原的第一性原理建模、原型双金属体系动力学的实验研究以及先进的原位结构表征方法。系统地研究各种铜基双金属表面的反应性将使用第一性原理方法进行。研究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。同时，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。第一性原理计算和实验努力的结合将导致对铜基双金属二氧化碳还原电催化剂结构-反应性相关性的基本见解和发展。此外，现场结构诊断工具将通过与国家实验室的科学家合作开发。这些工具将能够在现实条件下实时监测分子水平上的催化反应。这些支柱的整合将为焦博士长期从事多相催化研究奠定基础。

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.