Beyond Carbon Capture: Recycling CO2 to Decarbonize Steelmaking with Hydrogen and Photocatalysis
Precourt Pioneering Project
Awarded in the area of Hydrogen for Decarbonization. Award start date: August 1, 2022.
Background
Steel production today accounts for about 8% of global CO2 emissions. Steelmaking typically begins with ironmaking, in which iron oxide ores are successively reduced in blast furnaces with carbon monoxide into pig iron, generating CO2 in the process. Processed coal (coke) is used as the source of CO, and the resulting CO2 leads to the high carbon footprint of the process. This method still accounts for over 85% of the steel produced annually, so decarbonizing this process will be necessary to achieve emissions reductions goals of the future. In this work, a new strategy that uses hydrogen and solar-driven photochemical reduction of CO2 back into CO to produce water will be explored (see figure). This will help to decarbonize the blast furnace method of steel production.
Project Goal
This project aims to decarbonize 85% of steel extractions. To do this the team proposes a new CO2 recycling chamber that uses green hydrogen and plasmonic photocatalysis to regenerate carbon monoxide – the reducing fuel for ironmaking. The team will use computational methods to study catalysts, synthesize and characterize CO2-reducing nanoparticles, and optimize the reactions for performance in a reactor at laboratory scale. This approach will integrate advances in plasmonic photocatalysis, out-of-equilibrium chemical reactions, and green hydrogen into the ironmaking process. This project has the potential to significantly reduce CO2 emissions from the steelmaking industry with a scalable approach that builds on existing infrastructures. If this project is successful, it could lead to a new strategy to decarbonize existing blast furnaces through the use of hydrogen and solar-driven photochemistry.
Tasks and Timeline
The team aims to recycle CO2 in steelmaking to reduce the energy consumption and CO2 exhaust from both blast and shaft furnaces. The following tasks will be carried out:
- Computational design of plasmonic pathways for CO2 hydrogenation
The team will use computational methods to determine how the energy and spatial distribution of plasmons for the photocatalytic reduction of CO2 depend on the size (2–10 nm) and composition of the nanoparticles. These calculations will be experimentally validated using in situ transmission electron microscopy and spectroscopy in reactive CO2 environments.
- Characterize & scale the CO2 recycling:
The team will use a home-built photo-catalytic reactor to test the relationship between particle size, composition, illumination wavelength, and reaction performance – both in the CO2-recycling chamber and the iron oxide-reducing furnace.
- Connect CO2 recycling to optimal ore reduction:
The solid-gas chemistry of the iron ore reduction will be explored alongside optimization of the flue-gas reactor. A combination of electron and X-ray advanced characterization will map how the extent and kinetics of the 3-step reduction chemistry depend on the starting materials and flue gases. How candidate gas compositions (H2, CO2, and CO) change the kinetics of blast-furnace reaction will be resolved and how CO-dominated recycled gas changes the multiscale diffusional mechanisms of the reduction, will be understood to optimize the catalysts to maximize iron reduction.
Publications
1. L. Yuan, B. B. Bourgeois, C. C. Carlin, F. H. da Jornada, and J. A. Dionne. 2023. Sustainable Chemistry with Plasmonic Photocatalysts, Nanophotonics.
2. B. Bourgeois, C. Carlin, D. Angell, D. Swearer, W. Cheng, A. Dai, L. Yuan, J. Dionne. 2023. Linking Atomic and Reactor Scale Plasmon Photocatalysis in Acetylene Hydrogenation with Optically Coupled ETEM, Microscopy and Microanalysis.
3. A. R. Altman, S. Kundu, and F. H. da Jornada. 2023. Mixed Stochastic-Deterministic Approach for GW Calculations, Physical Review Letters.
4. C. C. Carlin, A. X. Dai, A. Al-Zubeidi, E. M. Simmerman, H. Oh, N. Gross, S. A. Lee, S. Link, C. F. Landes, F. H. da Jornada, and J. A. Dionne. 2023. Nanoscale and ultrafast in-situ techniques to probe plasmon photocatalysis, Chemical Physics Reviews.
5. X. Zheng, S. Paul, L. Moghimi, Y. Wang, R. A. Vilá, F. Zhang, X. Gao, J. Deng, Y. Jiang, X. Xiao, C. Wu, L. C. Greenburg, Y. Yang, Y. Cui, A. Vailionis, I. Kuzmenko, J. llavsky, Y. Yin, Y. Cui, and L. Dresselhaus-Marais. 2023. Correlating Chemical Reaction and Mass Transport in Hydrogen-Based Direct Reduction of Iron Oxide, PNAS.
Team Members
Felipe H. da Jornada
Felipe Jornada's research aims to predict and understand excited-state phenomena in quantum and energy materials. To make reliable predictions on novel materials, he relies on high-performance computer calculations based on parameter-free, quantum-mechanical theories developed in his group.
Leora Dresselhaus-Marais
Leora Dresselhaus-Marais studies how modern methods can enable new opportunities to update "old-school" materials processing and manufacturing for sustainability. This includes designing new microscopes and using them to get a deeper view into the extraction, forming, and functional properties of metallic materials.
Jennifer Dionne
Jennifer Dionne's research develops nanophotonic methods to observe and control chemical and biological processes as they unfold with nanometer-scale resolution, emphasizing critical challenges in global health and sustainability.
Xiaolin Zheng
Xiaolin Zheng's research focus is on the development and testing of novel materials for energy and propulsion applications.