Synthesis and Electronic Modulation of Nanostructured Layered Double Hydroxides for Efficient Electrochemical Oxygen Evolution.

Water electrolysis is considered to be one of the most promising technologies to produce clean fuels. However, its extensive realization critically depends on the progress in cost-effective and high-powered oxygen evolution reaction (OER) electrocatalysts. As a member of the big family of two-dimensional (2D) materials, nanostructured layered double hydroxides (nLDHs) have made significant processes and continuous breakthroughs for OER electrocatalysis. In this Review, the advancements in designing nLDHs for OER in recent years were discussed with a unique focus on their electronic modulations and in situ analysis on catalytic processes. After a brief discussion on different synthetic methodologies of nLDHs, including "bottom-up" and "top-down" approaches, the general strategies to enhance the catalytic performances of nLDHs reported so far were summarized, including compositional substitution, heteroatom doping, vacancy engineering, and amorphous/crystalline engineering. Furthermore, the in situ OER processes and mechanism analysis on engineering efficient nLDHs electrocatalysts were discussed. Finally, the research trends, perspectives, and challenges on designing nLDHs were also carefully outlined. This progress Review may offer enlightening experimental/theoretical guidance for designing highly catalytic active nLDHs and provide new directions to promote their future prosperity for practical utilization in water splitting.