4.8 Article

Design of Binary Cu-Fe Sites Coordinated with Nitrogen Dispersed in the Porous Carbon for Synergistic CO2 Electroreduction

Journal

SMALL
Volume 17, Issue 4, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202006951

Keywords

binary metal sites; CO2 reduction; DFT calculation; EXAFS analysis

Funding

  1. NSFC [21401004, 21701002, 21903001]
  2. Natural Science Foundation of Anhui Province [1508085QB36, 1908085QB58, 2008085MB52]
  3. Open Foundation of Anhui Laboratory of Molecule-Based Materials [fzj19005]
  4. Chemistry and Chemical Engineering Guangdong Laboratory [1911020]

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The designed Cu-Fe-N-6-C catalyst exhibits excellent performance with high selectivity and Faradaic efficiency towards CO, maintaining its high selectivity even after prolonged electrolysis. Synergistic catalysis of different metallic sites enhances CO2 adsorption enthalpy, reducing activation energy and resulting in high selectivity, activity, stability, and low impedance.
To relieve the green gas emission and involve the carbon neutral cycle, electrochemical reduction of CO2 attracts more and more attention. Herein, a biatomic site catalyst of Cu-Fe coordinated with the nitrogen, which is doped in the carbon matrix (denoted as Cu-Fe-N-6-C), is designed. The as-obtained Cu-Fe-N-6-C exhibits higher performance than that of Cu-N-C and Fe-N-C, owing to bimetallic sites, proving synergistic functions based on different molecules and their interfaces. Cu-Fe-N-6-C shows high selectivity toward CO, with high Faradaic efficiency (98% at -0.7 V), and maintaining 98% of its initial selectivity after 10 h electrolysis. The experimental results and theoretical calculations reveal that the synergistic catalysis of different metallic sites enlarges the adsorption enthalpy of CO2, reducing the activation energy result in generating high selectivity, activity, stability, and low impedance.

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