Science Highlight: Perlmutter Supports CO2 Fixation for Carbon-Negative Building Materials

Science Breakthrough

Researchers at Brookhaven National Laboratory and Columbia University used NERSC systems to advance their work on incorporating carbon dioxide (CO2) – a potent greenhouse gas – into carbon nanofibers (CNFs) that could be locked into construction materials and stored there for the lifetime of a building. Their work was published in Nature Catalysis in January.

Science Background

Carbon sequestration in reusable materials is a promising technology; however, carbon storage catalyzed through electrochemical, thermochemical, and other methods currently still allow carbon to leak into the atmosphere over time. To be truly carbon-neutral or carbon-negative, these methods would need to store the carbon on a more permanent basis.

Science Breakdown

Using both computer modeling and in situ experimentation, the researchers found that they could circumvent existing limitations of carbon storage by integrating the co-electrolysis of CO2 and water into CO and H2 with a separate thermochemical process at relatively low temperature (370–450 °C) and ambient pressure. The result fixed CO2 into CNF at a high rate of production; this combined strategy may provide a way to use renewable energy for decarbonizing CO2 into valuable solid carbon products while producing renewable H2, for an ultimately carbon-negative process.

The researchers used computer models to support their experimental processes and provide more detail on the chemical processes and results, and they used two NERSC systems to do it. First, they used Cori to perform spin-polarized density functional theory (DFT) calculations, then used the Vienna ab initio simulation package (VASP) to refine the work on Perlmutter. The DFT calculations enabled enhanced insights into the structures and catalytic behaviors observed experimentally — viewing the reactions atom by atom and confirming or explaining what they found. The computationally time-consuming but crucial calculations were important for mechanistic understanding and could not have taken place without support from NERSC.

Research Lead

Zhenhua Xie

Co-authors

Erwei Huang, Samay Garg, Sooyeon Hwang, Ping Liu, Jingguan G. Chen

Publication

Xie, Z., Huang, E., Garg, S. et al. “CO2 fixation into carbon nanofibres using electrochemical–thermochemical tandem catalysis.” Nat Catal 7, 98–109 (2024). https://doi.org/10.1038/s41929-023-01085-1

Funding

This work was financially supported by the U.S. Department of Energy Office of Science’s Office of Basic Energy Science, particularly the Division of Chemical Sciences, Geosciences and Biosciences.

User Facilities

National Energy Research Scientific Computing Center (NERSC)