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DATABASE GEO accession number GSE155778.We reported the selective electrochemical reduction of oxygen (O2 ) to hydroxyl radicals (. OH) via 3-electron pathway with FeCo alloy encapsulated by carbon aerogel (FeCoC). The graphite shell with exposed -COOH is conducive to the 2-electron reduction pathway for H2 O2 generation stepped by 1-electron reduction towards to . OH. The electrocatalytic activity can be regulated by tuning the local electronic environment of carbon shell with the electrons coming from the inner FeCo alloy. The new str