CAREER: Rational Design of Novel Electrocatalyst with Enhanced Properties

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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.