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Bixbyite-type Ln₂O₃ as promoters of metallic Ni for alkaline electrocatalytic hydrogen evolution.

ABSTRACT: The active-site density, intrinsic activity, and durability of Ni-based catalysts are critical to their application in industrial alkaline water electrolysis. This work develops a kind of promoters, the bixbyite-type lanthanide metal sesquioxides (Ln₂O₃), which can be implanted into metallic Ni by selective high-temperature reduction to achieve highly efficient Ni/Ln₂O₃ hybrid electrocatalysts toward hydrogen evolution reaction. The screened Ni/Yb₂O₃ catalyst shows the low overpotential (20.0 mV at 10 mA cm^-2), low Tafel slope (44.6 mV dec^-1), and excellent long-term durability (360 h at 500 mA cm^-2), significantly outperforming the metallic Ni and benchmark Pt/C catalysts. The remarkable hydrogen evolution activity and stability of Ni/Yb₂O₃ are attributed to that the Yb₂O₃ promoter with high oxophilicity and thermodynamic stability can greatly enlarge the active-site density, reduce the energy barrier of water dissociation, optimize the free energy of hydrogen adsorption, and avoid the oxidation corrosion of Ni.

SUBMITTER: Sun H

PROVIDER: S-EPMC9256667 | biostudies-literature | 2022 Jul

REPOSITORIES: biostudies-literature

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Bixbyite-type Ln2O3 as promoters of metallic Ni for alkaline electrocatalytic hydrogen evolution.

Sun Hongming H Yan Zhenhua Z Tian Caiying C Li Cha C Feng Xin X Huang Rong R Lan Yinghui Y Chen Jing J Li Cheng-Peng CP Zhang Zhihong Z Du Miao M

Nature communications 20220705 1

The active-site density, intrinsic activity, and durability of Ni-based catalysts are critical to their application in industrial alkaline water electrolysis. This work develops a kind of promoters, the bixbyite-type lanthanide metal sesquioxides (Ln2O3), which can be implanted into metallic Ni by selective high-temperature reduction to achieve highly efficient Ni/Ln2O3 hybrid electrocatalysts toward hydrogen evolution reaction. The screened Ni/Yb ...[more]

PMID: 35790749

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Project description:Efficient and cost-effective electrocatalysts for the hydrogen oxidation/evolution reaction (HOR/HER) are essential for commercializing alkaline fuel cells and electrolyzers. The sluggish HER/HOR reaction kinetics in base is the key issue that requires resolution so that commercialization may proceed. It is also quite challenging to decrease the noble metal loading without sacrificing performance. Herein, we report improved HER/HOR activity as a result of hydrogen spillover on platinum-supported MoO3 (Pt/MoO3-CNx-400) with a Pt loading of 20%. The catalyst exhibited a decreased over-potential of 66.8 mV to reach 10 mA cm-2 current density with a Tafel slope of 41.2 mV dec-1 for the HER in base. The Pt/MoO3-CNx-400 also exhibited satisfactory HOR activity in base. The mass-specific exchange current density of Pt/MoO3-CNx-400 and commercial Pt/C are 505.7 and 245 mA mgPt-1, respectively. The experimental results suggest that the hydrogen binding energy (HBE) is the key descriptor for the HER/HOR. We also demonstrated that the enhanced HER/HOR performance was due to the hydrogen spillover from Pt to MoO3 sites that enhanced the Volmer/Heyrovsky process, which led to high HER/HOR activity and was supported by the experimental and theoretical investigations. The work function value of Pt [Φ = 5.39 eV) is less than that of β-MoO3 (011) [Φ = 7.09 eV], which revealed the charge transfer from Pt to the β-MoO3 (011) surface. This suggested the feasibility of hydrogen spillover, and was further confirmed by the relative hydrogen adsorption energy [ΔGH] at different sites. Based on these findings, we propose that the H2O or H2 dissociation takes place on Pt and interfaces to form Pt-Had or (Pt/MoO3)-Had, and some of the Had shifted to MoO3 sites through hydrogen spillover. Then, Had at the Pt and interface, and MoO3 sites reacted with H2O and HO- to form H2 or H2O molecules, thereby boosting the HER/HOR activity. This work may provide valuable information for the development of hydrogen-spillover-based electrocatalysts for use in various renewable energy devices.

Dataset Information

Bixbyite-type Ln₂O₃ as promoters of metallic Ni for alkaline electrocatalytic hydrogen evolution.

Publications

Bixbyite-type Ln<sub>2</sub>O<sub>3</sub> as promoters of metallic Ni for alkaline electrocatalytic hydrogen evolution.

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