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Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d-Transition Metal Layered Double Hydroxides.

ABSTRACT: Layered double hydroxides (LDHs) are among the most active and studied catalysts for the oxygen evolution reaction (OER) in alkaline electrolytes. However, previous studies have generally either focused on a small number of LDHs, applied synthetic routes with limited structural control, or used non-intrinsic activity metrics, thus hampering the construction of consistent structure-activity-relations. Herein, by employing new individually developed synthesis strategies with atomic structural control, we obtained a broad series of crystalline α-M_A (II)M_B (III) LDH and β-M_A (OH)₂ electrocatalysts (M_A =Ni, Co, and M_B =Co, Fe, Mn). We further derived their intrinsic activity through electrochemical active surface area normalization, yielding the trend NiFe LDH > CoFe LDH > Fe-free Co-containing catalysts > Fe-Co-free Ni-based catalysts. Our theoretical reactivity analysis revealed that these intrinsic activity trends originate from the dual-metal-site nature of the reaction centers, which lead to composition-dependent synergies and diverse scaling relationships that may be used to design catalysts with improved performance.

SUBMITTER: Dionigi F

PROVIDER: S-EPMC8252729 | biostudies-literature |

REPOSITORIES: biostudies-literature

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