Collaborative Research: GCR: Non-Equilibrium Electrochemical Plasma Catalysis for Distributed Electrified Ammonia Synthesis

Ammonia is a potential hydrogen carrier for green power generation and enables long-duration energy storage and long-distance energy transport. Traditional large-scale ammonia synthesis using the Haber–Bosch process heavily relies on fossil fuel use and requires high-temperature and high-pressure catalysis, thus is both energy and carbon intensive and not suitable for distributed production. This project seeks to create a novel electrified, distributed, and efficient reactor to produce green ammonia with renewable electricity directly from nitrogen and water. Therefore, such reactors will not only provide a potential solution to decarbonization in chemical plants but also help address the challenges in the intermittency, regional dependence, and energy storage of renewable electricity. The project will also provide opportunities for young and underrepresented minority students to conduct collaborative research at universities and national laboratories. Moreover, it will contribute to US leadership in green manufacturing and nurture future US leaders and innovators in energy and chemical engineering sciences and technology. This GCR project will develop a new non-equilibrium electrochemical plasma catalysis (NE-EPC) system for efficient, distributed, electrified ammonia synthesis from water, nitrogen (N2), and renewable electricity. It will investigate a newly proposed non-equilibrium plasma assisted Mars−van Krevelen (PA-MvK) plasma catalysis mechanism. It will develop novel electrochemical membranes using cation and anion doped tungsten oxides for efficient proton intercalation and hydrogen atom transport as well as a ferroelectric plasma system with hybrid discharge to control atomic and vibrationally excited nitrogen generation to facilitate in situ membrane surface nitridation and efficient ammonia synthesis. Time resolved in situ diagnostics of plasma properties, electrons, atoms, and vibrationally excited molecules will be conducted using advanced laser diagnostic methods, such as femtosecond coherent anti-Stokes Raman scattering. The effect of surface crystalline structure, element ratios, N-vacancy sites, and mitigation on the NE-EPC reaction pathways will be examined by using atomic scale 4D scanning transmission electron microscopy and X-ray photoelectron spectroscopy. Experimentally validated quantum chemistry and machine learning modeling will also be developed to discover novel membrane materials and catalysts for NE-EPC. The project will provide a paradigm shift of fundamental science and technology innovation in non-equilibrium green chemical manufacturing. 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.