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Synthesis of hierarchical metal nanostructures with high electrocatalytic surface areas.

ABSTRACT: 3D interconnected structures can be made with molecular precision or with micrometer size. However, there is no strategy to synthesize 3D structures with dimensions on the scale of tens of nanometers, where many unique properties exist. Here, we bridge this gap by building up nanosized gold cores and nickel branches that are directly connected to create hierarchical nanostructures. The key to this approach is combining cubic crystal-structured cores with hexagonal crystal-structured branches in multiple steps. The dimensions and 3D morphology can be controlled by tuning at each synthetic step. These materials have high surface area, high conductivity, and surfaces that can be chemically modified, which are properties that make them ideal electrocatalyst supports. We illustrate the effectiveness of the 3D nanostructures as electrocatalyst supports by coating with nickel-iron oxyhydroxide to achieve high activity and stability for oxygen evolution reaction. This work introduces a synthetic concept to produce a new type of high-performing electrocatalyst support.

SUBMITTER: Gloag L

PROVIDER: S-EPMC9833653 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Synthesis of hierarchical metal nanostructures with high electrocatalytic surface areas.

Gloag Lucy L Poerwoprajitno Agus R AR Cheong Soshan S Ramadhan Zeno R ZR Adschiri Tadafumi T Gooding J Justin JJ Tilley Richard D RD

Science advances 20230111 2

3D interconnected structures can be made with molecular precision or with micrometer size. However, there is no strategy to synthesize 3D structures with dimensions on the scale of tens of nanometers, where many unique properties exist. Here, we bridge this gap by building up nanosized gold cores and nickel branches that are directly connected to create hierarchical nanostructures. The key to this approach is combining cubic crystal-structured cores with hexagonal crystal-structured branches in ...[more]

PMID: 36630515

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Project description:Compositionally versatile, nonstoichiometric, mixed ionic-electronic conducting metal oxides of the form A n+1B n O3n+1 (n = 1 → ∞; A = rare-earth-/alkaline-earth-metal cation; B = transition-metal (TM) cation) remain a highly attractive class of electrocatalysts for catalyzing the energy-intensive oxygen evolution reaction (OER). The current design strategies for describing their OER activities are largely derived assuming a static, unchanged view of their surfaces, despite reports of dynamic structural changes to 3d TM-based perovskites during OER. Herein, through variations in the A- and B-site compositions of A n+1B n O3n+1 oxides (n = 1 (A2BO4) or n = ∞ (ABO3); A = La, Sr, Ca; B = Mn, Fe, Co, Ni), we show that, in the absence of electrolyte impurities, surface restructuring is universally the source of high OER activity in these oxides and is dependent on the initial oxide composition. Oxide surface restructuring is induced by irreversible A-site cation dissolution, resulting in in situ formation of a TM oxyhydroxide shell on top of the parent oxide core that serves as the active surface for OER. The rate of surface restructuring is found to depend on (i) composition of A-site cations, with alkaline-earth-metal cations dominating lanthanide cation dissolution, (ii) oxide crystal phase, with n = 1 A2BO4 oxides exhibiting higher rates of A-site dissolution in comparison to n = ∞ ABO3 perovskites, (iii) lattice strain in the oxide induced by mixed rare-earth- and alkaline-earth-metal cations in the A-site, and (iv) oxide reducibility. Among the in situ generated 3d TM oxyhydroxide structures from A n+1B n O3n+1 oxides, Co-based structures are characterized by superior OER activity and stability, even in comparison to as-synthesized Co-oxyhydroxide, pointing to the generation of high active surface area structures through oxide restructuring. These insights are critical toward the development of revised design criteria to include surface dynamics for effectively describing the OER activity of nonstoichiometric mixed-metal oxides.

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Synthesis of hierarchical metal nanostructures with high electrocatalytic surface areas.

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Synthesis of hierarchical metal nanostructures with high electrocatalytic surface areas.

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