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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 | 2021 Jun

REPOSITORIES: biostudies-literature

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

Dionigi Fabio F Zhu Jing J Zeng Zhenhua Z Merzdorf Thomas T Sarodnik Hannes H Gliech Manuel M Pan Lujin L Li Wei-Xue WX Greeley Jeffrey J Strasser Peter P

Angewandte Chemie (International ed. in English) 20210526 26

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 cont ...[more]

PMID: 33844879

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Project description:High valence multi transition metal hydroxides are greatly enriched with OER redox active sites due to strong synergy of heteroatomic nuclei. The efficiency of these redox active sites could be efficiently improved by coupling with highly conductive substrate. The advanced three-dimensional (3D) architecture and hydrophilic terminal functionalities of MXene (MX) considerably enhance the maximum utilization rate of anchored redox active sites by triggering the direct growth of these at MX substrate. Here-in, the freeze-dried 3D network of crumpled Vanadium-Carbide (V2C) MX sheets regulates the crystallization of in-situ grown NiFeCr multi transition metal hydroxides on MX scaffold through co-precipitation process. The XPS results suggest a synergistic chemical interaction of 3D MX scaffold with NiFeCr that modifies the electronic structure of the composite ensuring reduced charge transfer resistance. Besides, as found in FESEM morphological investigation, the well-dispersed NiFeCr multi-transition metal hydroxides are immobilized on open pores like structure of V2C-MX facilitate thoroughly accessible active sites. As a result, the NiFeCr@3D V2C-MX composite has shown an excellent electrocatalytic activity with an overpotential of 410 mV at a current density of 200 mA cm-2, Tafel slope of 100 mV dec in 1M KOH. Besides, the significant interaction between metallic centers and MXene support prevent detachment or agglomeration of active centers providing maximum interaction with the electrolytic ions, quick ionic OH- transportation, speedy and stable electron transfer channels thus ensure the long-term stability of NV-5MX during 53 h continuous operation of OER. Furthermore, we have utilized a more accurate value of half-cell standard reduction potential of the Hg/HgO electrode in the Nernst equation to represent all test voltages and to determine the overpotential values. In essence, this study features a facile approach for the confined growth of multi transition metal hydroxides in the presence of morphologically unique 3D crumpled V2C MXene architectures. Consequently, the increased OER reaction kinetics and improved stability of the synthesized composites are potentially due to synergistic interplay between well dispersed active sites and the conductive substrate.

Dataset Information

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

Publications

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

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