NSF-BSF and Manufacturing USA: Lattice Oxygen Assisted Methane Activation for Modular Production of Fischer-Tropsch Ready Syngas

Methane from shale gas deposits has become an important energy resource. Methane is commercially used to produce hydrogen and liquid fuels via reforming and/or partial oxidation. Although significant efforts have been devoted to catalyst development, conventional methane reforming and partial oxidation processes are subjected to various intrinsic limitations. The proposed research aims to investigate a unique family of catalysts for partial oxidation of methane that are robust, active, and highly efficient. The project will be carried out jointly by the North Carolina State University research group and a group from the Blechner Center for Industrial Catalysis at the Ben-Gurion University of the Negev in Israel (Drs. Moti Herskowitz and Miron Landau).

The project team aims to design and characterize a class of core-shell redox catalysts that are both active methane partial oxidation (POx) catalysts and effective lattice oxygen (O2-) donors. The redox catalyst is composed of a transition metal oxide core for O2- storage, a mixed ionic-electronic conductive shell which facilitates O2-/electron conduction and inhibits primary oxide sintering/deactivation, and a tailored surface for methane partial oxidation. The catalyst is operated under a cyclic redox mode for methane POx (step 1) and lattice oxygen replenishment with air (step 2). The proposed research will investigate (i) O2- migration pathway in the redox catalyst and the phase compatibility between a number of core and shell materials; (ii) controlled synthesis and characterization of core-shell catalysts; (iii) active metal dispersion and reaction mechanism studies. (iv) kinetic modeling and demonstration of methane POx in a modular packed bed system. The proposed redox catalyst is unique since the embedded O2- allows effective methane oxidation without steam or oxygen. The active O2- also inhibits coke formation. The perovskite shell increases the sintering resistance of the primary oxide. It also provides an ideal surface for active metal dispersion and methane activation. Preliminary studies have led to core-shell redox catalysts with excellent oxygen storage capacity (20 w.t.%) and high syngas selectivity (>96%), activity (high syngas yields at 600 degrees C) and structural stability (tested up to 1,100 degrees C). In addition to training graduate and undergraduate students in research there are plans to engage high school students from underrepresented groups in STEM through outreach activities. The proposed project is responsive to the Manufacturing USA initiative and supports the mission of the DOE-funded RAPID Manufacturing Institute led by the American Institute of Chemical Engineers.

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.