Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 52, Pages 27324-27329Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202113895
Keywords
hierarchical porosity; metal organic frameworks; oxygen reduction reaction; zinc-air batteries
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Funding
- National Key Research and Development Program of China [2020YFB1506300]
- National Natural Science Foundation of China [21901019, 21625102, 21971017]
- Beijing Institute of Technology Research Fund Program
- Analysis and Testing Center of Beijing Institute of Technology
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Utilizing metal-organic frameworks (MOFs) as precursors, single-atom catalysts with high density have been successfully constructed. FeN4Cl1/NC demonstrates excellent oxygen reduction reaction (ORR) activity, with Cl optimizing the adsorption free energy of Fe sites to promote the ORR process.
The construction of single-atom catalysts (SACs) with high single atom densities, favorable electronic structures and fast mass transfer is highly desired. We have utilized metal-triazolate (MET) frameworks, a subclass of metal-organic frameworks (MOFs) with high N content, as precursors since they can enhance the density and regulate the electronic structure of single-atom sites, as well as generate abundant mesopores simultaneously. Fe single atoms dispersed in a hierarchically porous N-doped carbon matrix with high metal content (2.78 wt %) and a FeN4Cl1 configuration (FeN4Cl1/NC), as well as mesopores with a pore:volume ratio of 0.92, were obtained via the pyrolysis of a Zn/Fe-bimetallic MET modified with 4,5-dichloroimidazole. FeN4Cl1/NC exhibits excellent oxygen reduction reaction (ORR) activity in both alkaline and acidic electrolytes. Density functional theory calculations confirm that Cl can optimize the adsorption free energy of Fe sites to *OH, thereby promoting the ORR process. The catalyst demonstrates great potential in zinc-air batteries. This strategy selects, designs, and adjusts MOFs as precursors for high-performance SACs.
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