期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 37, 页码 16013-16022出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202007221
关键词
metal nanoclusters; metal-organic frameworks; oxygen evolution reaction; single atom catalyst; Zn-air battery
资金
- AIST
- JST Research Acceleration Programme
- JSPS-KAKENHI [JP16H06333, JP17H04797]
- Aichi Synchrotron Radiation Center [2019ND601, 2019ND602]
Understanding the thermal aggregation behavior of metal atoms is important for the synthesis of supported metal clusters. Here, derived from a metal-organic framework encapsulating a trinuclear Fe(2)(III)Fe(II)complex (denoted as Fe-3) within the channels, a well-defined nitrogen-doped carbon layer is fabricated as an ideal support for stabilizing the generated iron nanoclusters. Atomic replacement of Fe(II)by other metal(II) ions (e.g., Zn-II/Co-II) via synthesizing isostructural trinuclear-complex precursors (Fe2Zn/Fe2Co), namely the heteroatom modulator approach, is inhibiting the aggregation of Fe atoms toward nanoclusters with formation of a stable iron dimer in an optimal metal-nitrogen moiety, clearly identified by direct transmission electron microscopy and X-ray absorption fine structure analysis. The supported iron dimer, serving as cooperative metal-metal site, acts as efficient oxygen evolution catalyst. Our findings offer an atomic insight to guide the future design of ultrasmall metal clusters bearing outstanding catalytic capabilities.
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