The rational construction of amorphous-crystalline heterointerface can effectively improve the activity and stability of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, RuO/CoO (RCO) amorphous-crystalline heterointerface is prepared via oxidation method. The optimal RCO-10 exhibits low overpotentials of 57 and 231 mV for HER and OER at 10 mA cm, respectively. Experimental characterization and density functional theory (DFT) results show that the optimized electronic structure and surface reconstruction endow RCO-10 with excellent catalytic activity. DFT results show that electrons transfer from RuO to CoO through the amorphous-crystalline heterointerface, achieving electron redistribution and moving the d-band center upward, which optimizes the adsorption free energy of the hydrogen reaction intermediate. Moreover, the reconstructed Ru/Co(OH) during the HER process has low hydrogen adsorption free energy to enhance HER activity. The reconstructed RuO/CoOOH during the OER process has a low energy barrier for the elementary reaction (O*→*OOH) to enhance OER activity. Furthermore, RCO-10 requires only 1.50 V to drive 10 mA cm and maintains stability over 200 h for overall water splitting. Meanwhile, RCO-10 displays stability for 48 h in alkaline solutions containing 0.5 M NaCl. The amorphous-crystalline heterointerface may bring new breakthroughs in the design of efficient and stable catalysts.
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