Transition metal-based catalysts for electrochemical water splitting at high current density: current status and perspectives.

As a clean energy carrier, hydrogen has priority in decarbonization to build sustainable and carbon-neutral economies due to its high energy density and no pollutant emission upon combustion. Electrochemical water splitting driven by renewable electricity to produce green hydrogen with high-purity has been considered to be a promising technology. Unfortunately, the reaction of water electrolysis always requires a large excess potential, let alone the large-scale application (e.g., >500 mA cm needs a cell voltage range of 1.8-2.4 V). Thus, developing cost-effective and robust transition metal electrocatalysts working at high current density is imperative and urgent for industrial electrocatalytic water splitting. In this review, the strategies and requirements for the design of self-supported electrocatalysts are summarized and discussed. Subsequently, the fundamental mechanisms of water electrolysis (OER or HER) are analyzed, and the required important evaluation parameters, relevant testing conditions and potential conversion in exploring electrocatalysts working at high current density are also introduced. Specifically, recent progress in the engineering of self-supported transition metal-based electrocatalysts for either HER or OER, as well as overall water splitting (OWS), including oxides, hydroxides, phosphides, sulfides, nitrides and alloys applied in the alkaline electrolyte at large current density condition is highlighted in detail, focusing on current advances in the nanostructure design, controllable fabrication and mechanistic understanding for enhancing the electrocatalytic performance. Finally, remaining challenges and outlooks for constructing self-supported transition metal electrocatalysts working at large current density are proposed. It is expected to give guidance and inspiration to rationally design and prepare these electrocatalysts for practical applications, and thus further promote the practical production of hydrogen via electrochemical water splitting.