iScience (Apr 2024)

Precise regulation of phosphorus in nitrogen-coordinated porous carbon spheres for tunable CO2 electroreduction to syngas

  • Qi Xu,
  • Wentao Wang,
  • Yangyang Zhang,
  • Huanhuan Liu,
  • Xiaowen Wang,
  • Suyuan Zeng,
  • Genqiang Zhang

Journal volume & issue
Vol. 27, no. 4
p. 109470

Abstract

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Summary: The production of high-demand syngas with tunable ratios by CO2 electroreduction has attracted considerable research interest. However, it is challenging to balance the evolution performance of H2 and CO with wide H2/CO ratios, while maintaining high efficiency. Herein, nitrogen-coordinated hierarchical porous carbon spheres with varying phosphorus content (PxNC-T) are assembled to regulate syngas production performance. The precise introduction of P modulates the local charge distribution of nitrogen-coordinated carbons, thereby accelerating the protonation process of ∗CO2-to-∗COOH and promoting moderate H∗ adsorption. Specifically, syngas with wide H2/CO ratios (0.60–4.98) is obtained over a low potential range (−0.46 to −0.86 V vs. RHE). As a representative, P1.0NC-900 presents a remarkable current density (−152 mA cm−2) at −1.0 V vs. RHE in flow cells and delivers a decent peak power density (1.93 mW cm−2) in reversible Zn-CO2 batteries. Our work provides valuable insights into the rational design of carbon-based catalysts for CO2 reduction.

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