CATALYSIS SCIENCE INITIATIVE: From First Principles Design to Realization of Bimetallic Catalysts for Enhanced Selectivity

MAVRIKAKIS, MANOS DUMESIC, JAMES A.

关键词: CATALYSIS;    CATALYSTS;    DESIGN;    FUEL CELLS;    HYDROGEN PRODUCTION;    PRODUCTION;    SYNTHESIS GAS;    WATER GAS;    ALLOYS;    FISCHER-TROPSCH SYNTHESIS;    METHANOL;    METHANOL FUELS;    BIOFUELS catalysis;    surface science;    first-principles;    biofuels;   

DOI  :  10.2172/902903
RP-ID  :  NONE
PID  :  OSTI ID: 902903
Others  :  TRN: US200722%%334

学科分类：再生能源与代替技术

美国|英语

来源: SciTech Connect

【 摘 要 】

In this project, we have integrated state-of-the-art Density Functional Theory (DFT) models of heterogeneous catalytic processes with high-throughput screening of bimetallic catalytic candidates for important industrial problems. We have studied a new class of alloys characterized by a surface composition different from the bulk composition, and investigated their stability and activity for the water-gas shift reaction and the oxygen reduction reaction. The former reaction is an essential part of hydrogen production; the latter is the rate-limiting step in low temperature H2 fuel cells. We have identified alloys that have remarkable stability and activity, while having a much lower material cost for both of these reactions. Using this knowledge of bimetallic interactions, we have also made progress in the industrially relevant areas of carbohydrate reforming and conversion of biomass to liquid alkanes. One aspect of this work is the conversion of glycerol (a byproduct of biodiesel production) to synthesis gas. We have developed a bifunctional supported Pt catalyst that can cleave the carbon-carbon bond while also performing the water-gas shift reaction, which allows us to better control the H2:CO ratio. Knowledge gained from the theoretical metal-metal interactions was used to develop bimetallic catalysts that perform this reaction at low temperature, allowing for an efficient coupling of this endothermic reaction with other reactions, such as Fischer-Tropsch or methanol synthesis. In our work on liquid alkane production from biomass, we have studied deactivation and selectivity in these areas as a function of metal-support interactions and reaction conditions, with an emphasis on the bifunctionality of the catalysts studied. We have identified a stable, active catalyst for this process, where the selectivity and yield can be controlled by the reaction conditions. While complete rational design of catalysts is still elusive, this work demonstrates the power of combining the insights gained from theoretical models and the work of experiments to develop new catalysts for current and future industrial challenges.