A Highly Efficient Oxygen Evolution Catalyst Consisting of Interconnected Nickel–Iron‐Layered Double Hydroxide and Carbon Nanodomains

: In this work, a one-pot solution method for direct synthesis of interconnected ultrafine amorphous NiFe-layered double hydroxide (NiFe-LDH) (<5 nm) and nanocarbon using the molecular precursor of metal and carbon sources is presented for the first time. During the solvothermal synthesis of NiFe-LDH, the organic ligand decomposes and transforms to amorphous carbon with graphitic nanodomains by catalytic effect of Fe. The confined growth of both NiFe-LDH and carbon in one single sheet results in fully integrated amorphous NiFe-LDH/C nanohybrid, allowing the harness of the high intrinsic activity of NiFe-LDH due to (i) amorphous and distorted LDH structure, (ii) enhanced active surface area, and (iii) strong coupling between the active phase and carbon. As such, the resultant NiFe-LDH/C exhibits superior activity and stability. Different from postdeposition or electrostatic self-assembly process for the formation of LDH/C composite, this method offers one new opportunity to fabricate high-performance oxygen evolution reaction and possibly other catalysts.