Development of Sulfur and Carbon Tolerant Reforming Alloy Catalysts Aided Fundamental Atomistic Insights

Suljo Linic

关键词: ALLOYS;    CARBON;    CATALYSTS;    CURRENTS;    DENSITY;    DEPOSITS;    ERRORS;    FUNCTIONALS;    HYBRIDIZATION;    HYDROCARBONS;    LEAD;    MATERIALS;    METHANE;    OXIDATION;    POISONING;    POTENTIALS;    PROPANE;    STEAM;    SULFUR;    TOOLS;    TRANSFORMATIONS;   

DOI  :  10.2172/953215
RP-ID  :  None
PID  :  OSTI ID: 953215
Others  :  TRN: US201002%%1527

美国|英语

来源: SciTech Connect

【 摘 要 】

Current hydrocarbon reforming catalysts suffer from rapid carbon and sulfur poisoning. Even though there is a tremendous incentive to develop more efficient catalysts, these materials are currently formulated using inefficient trial and error experimental approaches. We have utilized a hybrid experimental/theoretical approach, combining quantum Density Functional Theory (DFT) calculations and various state-of-the-art experimental tools, to formulate carbon tolerant reforming catalysts. We have employed DFT calculations to develop molecular insights into the elementary chemical transformations that lead to carbon poisoning of Ni catalysts. Based on the obtained molecular insights, we have identified, using DFT quantum calculation, various Ni alloy catalysts as potential carbon tolerant reforming catalysts. The alloy catalysts were synthesized and tested in steam reforming and partial oxidation of methane, propane, and isooctane. We demonstrated that the alloy catalysts are much more carbon-tolerant than monometallic Ni catalysts under nearly stoichiometric steam-to-carbon ratios. Under these conditions, monometallic Ni is rapidly poisoned by sp2 carbon deposits. The research approach is distinguished by two characteristics: (a) knowledge-based, bottomup approach, compared to the traditional trial and error approach, allows for a more efficient and systematic discovery of improved catalysts. (b) the focus is on exploring alloy materials which have been largely unexplored as potential reforming catalysts.