Atomically Structured Metal-Organic Frameworks: A Powerful Chemical Path for Noble Metal-Based Electrocatalysts

Noble metal-based electrocatalysts (NMECs), particularly those with active sites at the nano or atomic level, are indispensable in heterogeneous catalysis, which has attracted considerable research interests, especially in the energy communities. Due to the enormous inherent merits, such as ultrahigh surface area, tunable atomic structure, and diverse chemical tailorability, metal-organic frameworks (MOFs) have been proposed as ideal candidates for creating efficient and programmable NMECs. In this review, from an interdisciplinary opinion,the recent progresses on the synthetic principles and catalytic site design protocols for the atomically structured MOFs and their derivatives are comprehensively discussed. Particularly, it is dedicated to summarizing the modulation strategies on creating the catalytic centers and bond microenvironments of MOFs-based NMECs, including the single-atom, dual-atom, cluster, and nanoparticle engineering. Furthermore, the critical mechanisms of how the structures of MOFs-based NMECs affect the corresponding electrochemical behaviors is outlined and disclose the critical essences for their future applications. Finally, the current developments, challenges, and perspectives for engineering the atomically structured MOFs-based NMECs are discussed to inspire the broad utilization of MOFs-based NMECs-equipped catalysts in energy conversion, which offers cutting-edge guidance for future prosperity in developing efficient NMECs. © 2023 Wiley-VCH GmbH.