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A restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation.

ABSTRACT: The development of highly efficient electrocatalysts for direct seawater splitting with bifunctionality for inhibiting anodic oxidation reconstruction and selective oxygen evolution reactions is a major challenge. Herein, we report a direct seawater oxidation electrocatalyst that achieves long-term stability for more than 1000 h at 600 mA/cm²@η₆₀₀ and high selectivity (Faraday efficiency of 100%). This catalyst revolves an amorphous molybdenum oxide layer constructed on the beaded-like cobalt oxide interface by atomic layer deposition technology. As demonstrated, a new restricted dynamic surface self-reconstruction mechanism is induced by the formation a stable reconstructed Co-Mo double hydroxide phase interface layer. The device assembled into a two-electrode flow cell for direct overall seawater electrolysis maintained at 1 A/cm²@1.93 V for 500 h with Faraday efficiency higher than 95%. Hydrogen generation rate reaches 419.4 mL/cm²/h, and the power consumption (4.62 KWh/m³ H₂) is lower than that of pure water (5.0 KWh/m³ H₂) at industrial current density.

SUBMITTER: Zhou L

PROVIDER: S-EPMC10954752 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature

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A restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation.

Zhou Ling L Guo Daying D Wu Lianhui L Guan Zhixi Z Zou Chao C Jin Huile H Fang Guoyong G Chen Xi'an X Wang Shun S

Nature communications 20240320 1

The development of highly efficient electrocatalysts for direct seawater splitting with bifunctionality for inhibiting anodic oxidation reconstruction and selective oxygen evolution reactions is a major challenge. Herein, we report a direct seawater oxidation electrocatalyst that achieves long-term stability for more than 1000 h at 600 mA/cm<sup>2</sup>@η<sub>600</sub> and high selectivity (Faraday efficiency of 100%). This catalyst revolves an amorphous molybdenum oxide layer constructed on the ...[more]

PMID: 38509067

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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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A restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation.

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A restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation.

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