Collaborative Research: Rational design of Ni/Ga intermetallic compounds for efficient light alkanes conversion through ammonia reforming

The transformation of cheap and abundant light alkanes (from natural gas) could have far-reaching implications on the chemical and energy sectors yet remains a formidable challenge due to the lack of efficient catalysts/catalytic systems. While various processes for alkane transformation to a host of petrochemical products have been extensively studied during the past decades, only steam methane reforming, propane dehydrogenation, and steam ethane noncatalytic cracking are produced at large-scale.

This project explores an alternative to current catalytic systems known as ammonia-assisted reforming (ammoreforming) of light alkanes. Ammoreforming involves reacting ammonia (NH3) with a light alkane (such as ethane, C3H8) to produce hydrogen cyanide (HCN – an important industrial chemical) and hydrogen (H2). Significantly, the reaction avoids production of either carbon monoxide or carbon dioxide, thus setting the stage for circular usage of carbon with minimal generation of greenhouse gas.

The project will strengthen academic research and educational programs in chemistry/chemical engineering at both Mississippi State University and Northern Illinois University. The project leverages several programs at both institutions aimed at stimulating K-12 students’ interest in STEM careers and providing underrepresented undergraduates opportunities to develop research skills.

The project focuses on the design and synthesis of efficient non-noble metal - NixGay intermetallic compound (IMC) based catalysts - by the understanding of the structure/performance relationships and catalytic mechanisms of the ammoreforming of light alkanes. The project focuses on several fundamental aspects of ammoreforming over the IMC catalysts, including (1) understanding the effect of oxalate precursor’s composition on the structure, surface properties, and particle size of the NixGay IMC catalysts and their relationships to the catalytic performance of ethane ammoreforming; (2) understanding the influence of oxalate thermo-decomposition and annealing on the structure and surface properties of the NixGay catalysts and the catalytic performance; (3) elucidating the reaction-induced surface/bulk reconstruction and identifying the surface reaction intermediates and catalytic mechanism.

The research will be carried out through the combination of in-situ/operando X-ray characterizations (including XRD, SAXS, and XAS) at the Advanced Photon Source of Argonne National Laboratory, operando-DRIFT-MS, and relaxation type transient experiments.

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.