Proceedings of nanoGe Fall Meeting19 (NFM19)
Publication date: 18th July 2019
Fuel cell technology and metal-air battery have attracted extensive interests from both academy and industry. Both of them require stable and effective precious metal-free electrocatalysts to replace noble metal-based benchmarks (such as Pt) for oxygen reduction reaction (ORR). In our work, phosphorus and nitrogen doping strategy has been used to co-coordinate with various transition atoms (e.g. Mn[1] and Fe[2]) on porosity- and morphology-engineered carbon support including mesoporous carbon and carbon hollow spheres. The as-prepared catalysts exhibit exceptional ORR activity in both alkaline and acidic electrolytes, which even outperform the commercial Pt/C under identical conditions. Based on X-ray absorption spectra and theoretical simulations, the extraordinary ORR performance of the catalysts can be ascribed to two main factors: i) Enhanced mesoporosity of carbon substrates by the introduction of phosphorus. The resulting large surface area and pore volume can facilitate the mass transfer and increases the number of exposed active sites. ii) The formation of N,P co-coordinated atomic-scale metal sites (MNxPy), which modifies the electronic configuration of the metal atoms and thereby boosts the ORR catalytic performance. The utilized approach in the work pave a new route to develop multi-heteroatoms coordinated metal sites embedded carbon composites toward cathodic ORR.
The work was supported by the Australian Research Council (ARC) under the Laurate Fellowship Scheme FL-140100081 and the Discovery Early Career Researcher Award DE170100375. We are thankful to Dr Wensheng Yan and the beamline of National Synchrotron Radiation Laboratory (Hefei, China) for the NEXAFS tests. We also thank Dr David Mitchell from the Electron Microscopy Centre, University of Wollongong, Australia, for his assistance in HAADF-STEM observations.
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