Issue 8, 2018

Boosting oxygen reduction catalysis with abundant copper single atom active sites

Abstract

With their high catalytic activity, stability, selectivity, and 100% atom utilization, single atomic non-noble metal based materials are valuable alternatives to efficient but expensive Pt based catalysts. For efficient catalysis, single-atom catalysts must expose abundant single atomic metal active centers. Here, we report the rational design and synthesis of a Cu single-atom catalyst with high Cu content of over 20.9 wt%, made of single atomic Cu anchored into an ultrathin nitrogenated two-dimensional carbon matrix (Cu–N–C). The high Cu content was achieved by the introduction of additional N species, which can securely trap and protect the Cu atoms. During oxygen reduction, the single atomic Cu exhibited over 54 times higher mass activity than metallic Cu nanoparticles at a potential of 0.85 V versus a reversible hydrogen electrode (RHE). Furthermore, the Cu–N–C exhibited 3.2 times higher kinetic current at 0.85 V (vs. RHE), and a much lower Tafel slope (37 mV dec−1), as well as better methanol/carbon monoxide tolerance and long-term stability than commercial Pt/C. Density functional theory (DFT) calculations reveal that the Cu active sites exhibit improved O–O bond stretching and favorable adsorption energies of O2 and OOH for four-electron oxygen reduction.

Graphical abstract: Boosting oxygen reduction catalysis with abundant copper single atom active sites

Supplementary files

Article information

Article type
Paper
Submitted
20 Apr 2018
Accepted
06 Jun 2018
First published
06 Jun 2018

Energy Environ. Sci., 2018,11, 2263-2269

Boosting oxygen reduction catalysis with abundant copper single atom active sites

F. Li, G. Han, H. Noh, S. Kim, Y. Lu, H. Y. Jeong, Z. Fu and J. Baek, Energy Environ. Sci., 2018, 11, 2263 DOI: 10.1039/C8EE01169A

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