Breaking the Hydrocarbon Cascade in Electric Process Heating: Strategies for Upgrading Fuel Gas Streams
In this work, we use plasma-catalysis to convert leftover methane (CH₄) and carbon dioxide (CO₂) in industrial flue gases (e.g., Fischer-Tropsch) into valuable fuels like methanol (MeOH). This approach tackles greenhouse gas emissions from fossil fuel heating while utilizing waste streams.
Summary of Research Outcomes
Energy yield: Currently 2.5 μg methanol/J but projected to reach 25 μg methanol /J with process optimization, surpassing conventional methods while achieving zero CO2 emissions.
Catalyst deactivation: A major challenge overcome by introducing H2 as a co-reactant, preventing oxidation and improving methanol selectivity from 8% to 24%, ~ 300% increase at ambient conditions.
Catalyst optimization: Tuning catalyst properties enhanced selectivity; copper exhibits 10 times higher performance than nickel.
Reaction mechanism: DRIFTS analysis reveals that copper facilitates CH3O* formation, a key precursor to methanol, through dissociative adsorption of CO2 and CH4.
Summary of Project Impacts
Electrified conversion: Converts unused fuel gas to valuable products at near ambient conditions.
Tunable selectivity: Achieves high selectivity for liquid fuels by adjusting plasma, gas phase, and catalyst properties.
Enhanced efficiency: Adding co-reactants improves selectivity to ~24% and increases overall efficiency
Principle Investigators
Team Members
Varanasi Sai Subhankar
Zachary Feng
Charan R Nallapareddy
Jiefeng Diao
Caroline C Leung
Graeme Henkelman
Project Publications
Tailoring Vibrational Excitation Pathways for High-Yield Oxidation of Methane to Methanol
Charan R Nallapareddy and Thomas C Underwood, ACS Sustainable Chemistry & Engineering
Controlling Catalytic Reaction Pathways with Plasma-activated Co-reactants for Selective Liquid Fuel Extraction
Varanasi Sai Subhankar, C. Buddie Mullins, Thomas C Underwood, and Michael Baldea