Journal
NANOSCALE
Volume 11, Issue 30, Pages 14266-14275Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9nr04156g
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Funding
- Korean Ministry of Science and ICT [2014R1A6A1030732, 2017K000494, 2017H1D3A1A01014082, 2018R1A2B6003634, 2018R1A2B2006474]
- National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information [KSC-2018-CRE-0067]
- Korea University
- Jeonju University
- KBSI RD program [D39700]
- National Research Foundation of Korea [2017H1D3A1A01014082, 2018R1A2B6003634] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Two-dimensional (2D) MoS2 nanostructures have been extensively investigated in recent years because of their fascinating electrocatalytic properties. Herein, we report 2D hybrid nanostructures consisting of 1T ' phase MoS2 and Fe-phthalocyanine (FePc) molecules that exhibit excellent catalytic activity toward both the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). X-ray absorption spectra revealed an increased Fe-N distance (2.04 angstrom) in the hybrid complex relative to the isolated FePc. Spin-polarized density functional theory calculations predicted that the Fe center moves toward the MoS2 layer and induces a non-planar structure with an increased Fe-N distance of 2.05 angstrom, which supports the experimental results. The experiments and calculations consistently show a significant charge transfer from FePc to stabilize the hybrid complex. The excellent HER catalytic performance of FePc-MoS2 is characterized by a low Tafel slope of 32 mV dec(-1) at a current density of 10 mA cm(-2) and an overpotential of 0.123 V. The ORR catalytic activity is superior to that of the commercial Pt/C catalyst in pH 13 electrolyte, with a more positive half-wave potential (0.89 vs. 0.84 V), a smaller Tafel slope (35 vs. 87 mV center dot dec(-1)), and a much better durability (9.3% vs. 40% degradation after 20 h). Such remarkable catalytic activity is ascribed to the HER-active 1T ' phase MoS2 and the ORR-active nonplanar Fe-N-4 site of FePc.
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