期刊
ACS CATALYSIS
卷 11, 期 15, 页码 9355-9365出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c02434
关键词
oxygen reduction reaction; highly ordered Pt alloy nanoparticles; direct thermal annealing synthesis; N-doped carbon shell; single-wall carbon nanohorns
资金
- National Natural Science Foundation of China [21771184, 51872048]
- STS project of Fujian Province [2018T3004]
Using a two-step direct annealing method, uniform and ordered PtFe alloy nanoparticles were synthesized on single-wall carbon nanohorns (SWCNHs), demonstrating excellent catalytic performance for the oxygen reduction reaction (ORR). The sample exhibited uniform face-centered tetragonal (fct) structure PtFe nanoparticles on the SWCNH support, maintaining high catalytic activity even after long-term stability test.
Ordered Pt alloy electrocatalysts supported on carbon nanomaterials have attracted widespread attention, especially for the oxygen reduction reaction (ORR), due to the catalytic performance derived from their unique electronic and geometric structures. However, it is still urgent to fabricate uniform and structurally ordered Pt alloy electrocatalysts based on simple methods. Herein, a two-step direct annealing method was applied to synthesize uniform and ordered PtFe alloy nanoparticles loaded on single-wall carbon nanohorns (SWCNHs) under the protection of a thin N-doped carbon (NC) shell, which was in situ generated from the polymerization and pyrolysis of a small organic ligand, namely, aniline, during the first annealing treatment. After the second annealing treatment in a H-2 atmosphere for 9 h, the obtained sample, denoted as PtFe@NC/SWCNHs(H-2-9h), exhibited uniform and ordered PtFe nanoparticles with a face-centered tetragonal (fct) structure (ordered degree: >80%, mean size: similar to 5.2 nm) on the graphitic SWCNH support. Without removing the NC shell, the PtFe@NC/SWCNHs(H-2-9h) sample showed mass activity (1.53 A/mg(Pt) at 0.9 V) and specific activity (3.61 mA/cm(2) at 0.9 V) toward the ORR due to the enhanced electronic interaction derived from the ordered fct-PtFe structure. Importantly, it still retained high catalytic activity after a long-term stability test, mainly owing to the ordered fct-PtFe structure and the protection of the NC shell, which provides strong resistance toward the Fe leaching and nanoparticle aggregation, respectively. The presented strategy is generalized to fabricate different ordered PtM or Pt3M (M = Fe/Co) alloy electrocatalysts.
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