期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 23, 期 10, 页码 2255-2260出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201605337
关键词
2D materials; active sites; hydrogen evolution reaction; metal-organic frameworks; single-layer nanosheet
资金
- ERC
- EC [CNECT-ICT-604391]
- Alexander von Humboldt-Foundation
- Marie-Curie Fellowship [CONJUGATION-706082]
Carbon electrocatalysts consisting of metal complexes such as MNx or MSx are promising alternatives to high-cost Pt catalysts for the hydrogen evolution reaction (HER). However, the exact HER active sites remain elusive. Here, molecular metal dithiolene-diamine (MS2N2, M=Co and Ni), metal bis(dithiolene) (MS4), and metal bis(diamine) (MN4) complexes were selectively incorporated into carbon-rich 2D metal-organic frameworks (2D MOFs) as model carbon electrocatalysts. The 2D MOF single layers, powders, and composites with graphene were thus prepared and showed definite active sites for H-2 generation. The electrocatalytic HER activity of the 2D MOF-based catalysts with different metal complexes follow the order of MS2N2 > MN4 > MS4. Moreover, the protonation preferentially occurred on the metal atoms, and the concomitant heterolytic elimination of H-2 was favored on the M-N units in the MS2N2 active centers. The results provide an in-depth understanding of the catalytic active sites, thus making way for the future development of metal complexes in carbon-rich electrode materials for energy generation.
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