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DOI10.1039/c8ee01169a
Boosting oxygen reduction catalysis with abundant copper single atom active sites
Li F.; Han G.-F.; Noh H.-J.; Kim S.-J.; Lu Y.; Jeong H.Y.; Fu Z.; Baek J.-B.
发表日期2018
ISSN17545692
起始页码2263
结束页码2269
卷号11期号:8
英文摘要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. © 2018 The Royal Society of Chemistry.
英文关键词Atoms; Catalysis; Catalyst activity; Catalyst selectivity; Density functional theory; Design for testability; Electrolytic reduction; Oxygen; Precious metals; Slope stability; Adsorption energies; Atom utilization; Kinetic currents; Long term stability; Metallic Cu nanoparticles; Oxygen reduction catalysis; Pt-based catalyst; Reversible hydrogen electrodes; Copper; adsorption; catalysis; catalyst; copper; electrode; electron; oxygen; reduction
语种英语
来源期刊Energy & Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/190155
作者单位School of Energy and Chemical Engineering, Center for Dimension-Controllable Organic Frameworks, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST, Ulsan, 44919, South Korea; CAS, Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China (USTC), Hefei, 230026, China; Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China (USTC), Hefei, 230026, China; National Synchrotron Radiation Laboratory, University of Science and Technology of China (USTC), Hefei, 230026, China; UNIST Central Research Facilities, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST, Ulsan, 44919, South Korea
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GB/T 7714
Li F.,Han G.-F.,Noh H.-J.,et al. Boosting oxygen reduction catalysis with abundant copper single atom active sites[J],2018,11(8).
APA Li F..,Han G.-F..,Noh H.-J..,Kim S.-J..,Lu Y..,...&Baek J.-B..(2018).Boosting oxygen reduction catalysis with abundant copper single atom active sites.Energy & Environmental Science,11(8).
MLA Li F.,et al."Boosting oxygen reduction catalysis with abundant copper single atom active sites".Energy & Environmental Science 11.8(2018).
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