Bimetallic Nickel‐Substituted Cobalt‐Borate Nanowire Array: An Earth‐Abundant Water Oxidation Electrocatalyst with Superior Activity and Durability at Near Neutral pH

There is an urgent demand to develop earth‐abundant electrocatalysts for efficient and durable water oxidation under mild conditions. A nickel‐substituted cobalt‐borate nanowire array is developed on carbon cloth (Ni‐Co‐Bi/CC) via oxidative polarization of NiCo 2 S 4 nanoarray in potassium borate (K‐Bi). As a bimetallic electrocatalyst for water oxidation, such Ni‐Co‐Bi/CC is superior in catalytic activity and durability in 0.1 m K‐Bi (pH: 9.2), with a turnover frequency of 0.33 mol O 2 s −1 at the overpotential of 500 mV and nearly 100% Faradaic efficiency. To drive a geometrical catalytic current density of 10 mA cm −2 , it only needs overpotential of 388 mV, 34 mV less than that for Co‐Bi/CC, outperforming reported non‐noble‐metal catalysts operating under benign conditions. Notably, its activity is maintained over 80 000 s. Density functional theory calculations suggest that the O* to OOH* conversion is the rate‐determining step and Ni substitution decreases the free energy on Co‐Bi from 2.092 to 1.986 eV.