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Circumventing thermodynamic limitations in converting carbon dioxide into carbon nanotubes via tandem catalysis

| Source: PNAS

Carbon nanotubes (CNTs) are important materials for electronics and structural composites, but their production still relies on hydrocarbon-based chemical vapor deposition, an energy-intensive and fossil-dependent process, limited by rapid catalyst deactivation. Using CO 2 as a carbon feedstock offers a sustainable route for CNT synthesis, yet direct CO 2 conversion to CNTs is thermodynamically unfavorable and existing CO 2 -to-carbon pathways mainly yield amorphous or weakly graphitized solids.

Carbon nanotubes (CNTs) are important materials for electronics and structural composites, but their production still relies on hydrocarbon-based chemical vapor deposition, an energy-intensive and fossil-dependent process, limited by rapid catalyst deactivation. Using CO 2 as a carbon feedstock offers a sustainable route for CNT synthesis, yet direct CO 2 conversion to CNTs is thermodynamically unfavorable and existing CO 2 -to-carbon pathways mainly yield amorphous or weakly graphitized solids. Here, we demonstrate a tandem electrochemical–thermochemical (EC-TC) strategy that overcomes these limitations. CO 2 is first electrochemically reduced to a tunable mixture of C 2 H 4 and CO, which is directly fed into a thermochemical reactor and converted into CNTs with controllable morphology and high CNT-to-metal mass ratios (~200) over NiFe catalysts at 750 °C. In situ synchrotron-based characterization and density functional theory calculations reveal that CO dissociation and C 2 H 4 decomposition on NiFe alloys cooperatively promote CNT nucleation and sustained growth. This EC-TC strategy establishes a modular route for converting CO 2 into value-added carbon nanomaterials.

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