<p>Upgrading decentralized biogas represents a sustainable route to produce valuable products while mitigating two potent greenhouse gases, namely, methane (CH<sub>4</sub>) and carbon dioxide (CO<sub>2</sub>). Conventional dry reforming of CH<sub>4</sub> with CO<sub>2</sub> yields syngas with low H<sub>2</sub>/CO ratios (≤1) and requires high temperatures (&gt;800 °C) to overcome equilibrium constraints and abate coke deposition, which limits commercial implementation. Here we demonstrate the conversion of biogas into value-added carbon nanofibers via reaction integration in tandem reactors, while reducing the reaction temperature, shifting equilibrium limits and yielding H<sub>2</sub>-enriched syngas (H<sub>2</sub>/CO = 2–3) as a byproduct. Experimental and theoretical insights reveal that potassium (K) modification enhances carbon nanofiber formation due to synergistic effects via a balanced interplay between KO<sub><i>x</i></sub>-induced cobalt facets and cobalt carbide species. The energy cost and CO<sub>2</sub> footprint analyses highlight the potential advantages of tandem processes for the sustainable upgrading of biogas into valuable solid carbon products.</p><p></p>

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Biogas sequestration to carbon nanofibers via tandem catalytic strategies

  • Zhenhua Xie,
  • Erwei Huang,
  • Kevin K. Turaczy,
  • Samay Garg,
  • Sooyeon Hwang,
  • Prabhakar Reddy Kasala,
  • Ping Liu,
  • Jingguang G. Chen

摘要

Upgrading decentralized biogas represents a sustainable route to produce valuable products while mitigating two potent greenhouse gases, namely, methane (CH4) and carbon dioxide (CO2). Conventional dry reforming of CH4 with CO2 yields syngas with low H2/CO ratios (≤1) and requires high temperatures (>800 °C) to overcome equilibrium constraints and abate coke deposition, which limits commercial implementation. Here we demonstrate the conversion of biogas into value-added carbon nanofibers via reaction integration in tandem reactors, while reducing the reaction temperature, shifting equilibrium limits and yielding H2-enriched syngas (H2/CO = 2–3) as a byproduct. Experimental and theoretical insights reveal that potassium (K) modification enhances carbon nanofiber formation due to synergistic effects via a balanced interplay between KOx-induced cobalt facets and cobalt carbide species. The energy cost and CO2 footprint analyses highlight the potential advantages of tandem processes for the sustainable upgrading of biogas into valuable solid carbon products.