Journal
NANO RESEARCH
Volume 16, Issue 2, Pages 1869-1877Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4979-x
Keywords
manganese (Mn)-iron (Fe) binuclear sites; synergistic effect; spin state; oxygen reduction reaction
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In this study, dual-metal atomic pairs of Mn-Fe binuclear sites anchored onto a graphite-like structure were constructed. The strong short-range electronic interaction between Mn and Fe sites in the binuclear structure transforms Fe sites to a high spin state, improving the oxygen reduction reaction performance of the Mn-Fe structure.
In this study, dual-metal atomic pairs of manganese (Mn)-iron (Fe) binuclear sites (BNSs) with two conjoint MnN4 and FeN4 moieties (MnFeN8) anchored onto a graphite-like structure (GLS) (Mn-Fe BNSsIGLS) were constructed. The binuclear MnFeN8 structure was verified experimentally and theoretically. Magnetic measurements and Gaussian calculations reveal that this unique Mn-Fe BNSs exhibit strong short-range electronic interaction between Mn and Fe sites, which decouples two paired d electrons in Fe sites, thereby transforming Fe sites from an intermediate to a high spin state. The optimal electronic configuration of Fe sites and their binuclear structure facilitate an oxygen reduction reaction (ORR) thermodynamically and dynamically, respectively, endowing Mn-Fe BNSs with improved ORR performance.
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