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Electrochemical water splitting is considered as the sustainable, environmentalfriendly and low-cost technology for renewable energy supplement. [6,7] Pt and Ir (or Ru)-based nanocrystals are the best metal catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, in overall water splitting device, [8][9][10][11] but unfortunately, their further applications are still hindered by their poor intrinsic electrocatalytic activities resulting from sluggish kinetics of HER and OER. [6,7] Pt and Ir (or Ru)-based nanocrystals are the best metal catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, in overall water splitting device, [8][9][10][11] but unfortunately, their further applications are still hindered by their poor intrinsic electrocatalytic activities resulting from sluggish kinetics of HER and OER.