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A highly efficient atomically thin curved PdIr bimetallene electrocatalyst.

ABSTRACT: The multi-metallene with an ultrahigh surface area has great potential in precise tuning of surface heterogeneous d-electronic correlation by surface strain effect for the distinctive surface electronic structure, which is a brand new class of promising 2D electrocatalyst for sustainable energy device application. However, achieving such an atomically thin multi-metallene still presents a great challenge. Herein, we present a new synthetic method for an atomic-level palladium-iridium (PdIr) bimetallene with an average thickness of only ∼1.0 nm for achieving superior catalysis in the hydrogen evolution reaction (HER) and the formic acid oxidation reaction (FAOR). The curved PdIr bimetallene presents a top-ranked high electrochemical active area of 127.5 ± 10.8 m² g_Pd+Ir ^-1 in the reported noble alloy materials, and exhibits a very low overpotential, ultrahigh activity and improved stability for HER and FAOR. DFT calculation reveals that the PdIr bimetallene herein has a unique lattice tangential strain, which can induce surface distortion while concurrently creating a variety of concave-convex featured micro-active regions formed by variously coordinated Pd sites agglomeration. Such a strong strain effect correlates the abnormal on-site active 4d¹⁰-t_2g-orbital Coulomb correlation potential and directly elevates orbital-electronegativity exposure within these active regions, resulting in a preeminent barrier-free energetic path for significant enhancement of FAOR and HER catalytic performance.

SUBMITTER: Lv F

PROVIDER: S-EPMC8433090 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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A highly efficient atomically thin curved PdIr bimetallene electrocatalyst.

Lv Fan F Huang Bolong B Feng Jianrui J Zhang Weiyu W Wang Kai K Li Na N Zhou Jinhui J Zhou Peng P Yang Wenxiu W Du Yaping Y Su Dong D Guo Shaojun S

National science review 20210202 9

The multi-metallene with an ultrahigh surface area has great potential in precise tuning of surface heterogeneous d-electronic correlation by surface strain effect for the distinctive surface electronic structure, which is a brand new class of promising 2D electrocatalyst for sustainable energy device application. However, achieving such an atomically thin multi-metallene still presents a great challenge. Herein, we present a new synthetic method for an atomic-level palladium-iridium (PdIr) bime ...[more]

PMID: 34691734

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Project description:The efficient electrocatalysts for direct methanol oxidation play an essential role in the electrochemical energy conversion systems for their application in a wide range of portable applications. Consequently, Cu-doped NiO thin films on fluorine-doped tin oxide (FTO) were successfully prepared by the co-sputtering deposition technique, using various deposition times (300, 600, 900, and 1200 seconds), and producing films of different thicknesses (30, 55, 90, and 120 nm, respectively). X-ray diffraction (XRD) revealed the ideal crystallinity of the structure of the prepared films and was used to observe the effect of the thickness of the films on the crystal size. Energy-dispersive X-ray spectroscopy (EDS) confirmed the purity of the deposited film without any contamination. Field emission scanning electron microscopy (FESEM) images confirmed the film thickness increase with increasing deposition time. The surface roughness value of the Cu-NiO 1200 film was found to be 3.2 nm based on the atomic force microscopy (AFM) measurements. The deposited thin films of different thicknesses have been used as electrocatalysts for methanol oxidation at various concentrations of methanol (0, 0.5, 1, and 2 M), and displayed the highest electrocatalytic performance in 1 M methanol. Cu-doped NiO thin films have the advantage as electrocatalysts where they can be used directly without adding any binder or conducting agents, this is because Cu-doped NiO is deposited with high adhesion and strong electrical contact to the FTO substrate. A clear impact on the catalytic activity with increasing film thickness and a correlation between the film thickness and its catalytic activity was observed. The current density increased by about 60% for the Cu-NiO 1200 sample compared to Cu-NiO 300 sample, with the lowest onset potential of 0.4 V vs. Ag/AgCl. All deposited thin films of different thicknesses exhibited high stability at 0.6 V in 1 M methanol. This will open the window toward using physical deposition techniques for optimizing the electrocatalytic activity of different catalysts for electrocatalytic applications.

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A highly efficient atomically thin curved PdIr bimetallene electrocatalyst.

Publications

A highly efficient atomically thin curved PdIr bimetallene electrocatalyst.

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