Mild Construction of “Midas Touch” Metal–Organic Framework‐Based Catalytic Electrodes for Highly Efficient Overall Seawater Splitting

Abstract Mild construction of highly efficient and durable practical electrodes for overall water splitting (OWS) at industrial‐grade current density is currently a significant challenge. Herein, metal–organic framework (MOF) materials are grown in situ on the surface of carbon cloth (CC) at 25 °C, and quickly “interspersed” by cobalt–boron (Co–B) via electroless plating for 30 min to obtain a highly efficient and stable CoB@MOF@CC self‐supporting electrode. Owing to the large specific surface area, abundant active sites, and porous structure, the MOF‐based CC modified by bamboo leaf‐like ultrathin CoB has remarkable electrochemical catalysis efficiency. The CoB@MOF@CC electrode exhibits excellent performance during the hydrogen evolution reaction (η 10 = 57 mV, η 500 = 266 mV) and oxygen evolution reaction (η 10 = 209 mV, η 500 = 423 mV) in alkaline simulated seawater, and is durable for 2500 h at 500 mA cm −2 . The OWS performance is obviously enhanced by employing the prepared electrode, which only requires 1.49 V to achieve 10 mA cm −2 and is durable for over 360 h at industrial‐grade current densities in alkaline high‐salt, real seawater, rainwater, and urea electrolytes.