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Modulating the electronic metal‐support interaction (EMSI) of the single‐atomic sites against leaching via microenvironment regulation is critical to achieving high activity and stability but remains challenging. Herein, this work selectively confines Pt single atoms on CoFe layered double hydroxide (LDH) by three oxygen atoms around cation vacancy (Pt1/LDHV) or one oxygen atom at the regular surface...