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Enhanced reduction of nitrate by noble metal-free electrocatalysis on P doped three-dimensional Co3O4 cathode: Mechanism exploration from both experimental and DFT studies

Gao, Jianan ; Jiang, Bo ; Ni, Congcong ; Qi, Yuanfeng ; Bi, Xuejun

Chemical engineering journal (Lausanne, Switzerland : 1996), 2020-02, Vol.382, p.123034, Article 123034 [Periódico revisado por pares]

Elsevier B.V

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  • Título:
    Enhanced reduction of nitrate by noble metal-free electrocatalysis on P doped three-dimensional Co3O4 cathode: Mechanism exploration from both experimental and DFT studies
  • Autor: Gao, Jianan ; Jiang, Bo ; Ni, Congcong ; Qi, Yuanfeng ; Bi, Xuejun
  • Assuntos: Atomic hydrogen ; Electrochemical denitrification ; Indirect reduction ; Non-precious catalyst ; P-Co3O4/NF cathode
  • É parte de: Chemical engineering journal (Lausanne, Switzerland : 1996), 2020-02, Vol.382, p.123034, Article 123034
  • Descrição: [Display omitted] •P-Co3O4/NF cathode was prepared for the electrochemical reduction of nitrate.•The production and adsorption of atomic H* were enhanced on Co3O4 surface after P doping.•The indirect reduction of nitrate mediated by atomic H* was boosted.•The N2 selectivity and TN removal efficiency were increased with elevating Cl− concentration. Developing green, sustainable and economical materials for emerging electrochemical remediation of nitrate (NO3−) contaminant have attracted immense research interest. In this study, a cost-effective and stable three-dimensional P-doped Co3O4/nickel foam (NF) was prepared for electrocatalytic reduction of NO3− in water. The doping of P could replace the lattice oxygen in Co3O4 and lead to the enhancements in Co3+ percentage and empty d orbitals. As a result, the relative energy for Volmer reaction and the adsorption energy of atomic H* decreased to be −0.73 eV and −3.60 eV, respectively. Furthermore, the higher electrochemical active area and lower interface impedance of Co3O4 were attained after P doping. The P2.1-Co3O4/NF cathode outperformed Co3O4/NF in the NO3− reduction rate (8.45 times faster) and contribution of atomic H* (2.37 folds increase in the ratio). And almost 100% N2 selectivity can be obtained in the presence of 2500 mg L−1 chloride ions. Generally, this study provided a new paradigm for designing more practical non-metallic catalyst for NO3− reduction.
  • Editor: Elsevier B.V
  • Idioma: Inglês
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  • Realização: ABCD-USP USP   Logos de Redes Sociais: Freepik

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