The Underlying Molecular Mechanism of Fence Engineering to Break the Activity–Stability Trade‐Off in Catalysts for the Hydrogen Evolution Reaction

Hao, Mengyao; Mao, Baoguang; Zheng, Lirong; Zhu, Jie; Cao, Minhua

doi:10.1002/ange.202114899

Cited by 5 publications

(2 citation statements)

References 55 publications

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“…69 ). This suggests that the Ni phase in Ni/Yb 2 O 3 is more resistant to O 2 interaction and oxidation erosion than pure Ni 63 , which ensures the highly active heterojunction of Ni and Yb 2 O 3 during the HER process. Moreover, the lowered H binding energy on Ni of Ni/Yb 2 O 3 can decrease the hydrogen-adsorption poison of Ni active sites, thus improving its long-term stability for HER 64 .…”

Section: Resultsmentioning

confidence: 99%

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

et al. 2022

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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.

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Section: Resultsmentioning

confidence: 99%

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

et al. 2022

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“…Electrocatalysis can efficiently convert raw materials into chemicals by renewable electricity, which attracts great attention in recent years 1 , 2 . However, electrode/catalyst deterioration is a common problem that reduces catalytic efficiency and further results in additional costs 3 , 4 . Traditional electrocatalysts are loaded on rigid current collectors (e.g., glassy carbon, carbon paper, and foamed metal) and decay in their catalytic performance by sintering, poisoning, spoilage, or losing active sites during the long-term process (Fig.…”

Section: Introductionmentioning

confidence: 99%

A self-healing electrocatalytic system via electrohydrodynamics induced evolution in liquid metal

et al. 2022

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Catalytic deterioration during electrocatalytic processes is inevitable for conventional composite electrodes, which are prepared by depositing catalysts onto a rigid current collector. In contrast, metals that are liquid at near room temperature, liquid metals (LMs), are potential electrodes that are uniquely flexible and maneuverable, and whose fluidity may allow them to be more adaptive than rigid substrates. Here we demonstrate a self-healing electrocatalytic system for CO2 electroreduction using bismuth-containing Ga-based LM electrodes. Bi2O3 dispersed in the LM matrix experiences a series of electrohydrodynamic-induced structural changes when exposed to a tunable potential and finally transforms into catalytic bismuth, whose morphology can be controlled by the applied potential. The electrohydrodynamically-induced evolved electrode shows considerable electrocatalytic activity for CO2 reduction to formate. After deterioration of the electrocatalytic performance, the catalyst can be healed via simple mechanical stirring followed by in situ regeneration by applying a reducing potential. With this procedure, the electrode’s original structure and catalytic activity are both recovered.

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Boosting the Stability of Oxygen Vacancies in α‐Co(OH)₂ Nanosheets with Coordination Polyhedrons as Rivets for High‐Performance Alkaline Hydrogen Evolution Electrocatalyst

Jiang

Huang

Zou

et al. 2022

Advanced Energy Materials

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The strong alkaline electrolytes are utilized in various key electrochemical applications and the severe corrosion by hydroxyl ions endows the development of high‐performance electrode materials with a great challenge. Here, an effective strategy is demonstrated to stabilize α‐Co(OH)2 under harsh alkaline electrochemical condition by coordination polyhedron pinning (MoO42−, WO42−) on the surface for hydrogen evolution reaction (HER). The addition of MoO42− in 1 m KOH can inhibit the attack of hydroxyl ions on oxygen vacancies in α‐Co(OH)2, and simultaneously modulate the electronic structure of active sites for HER. The theoretical calculations and experimental results reveal that MoO42− can be riveted on the surface of α‐Co(OH)2 to greatly stabilize oxygen vacancies and inhibit the formation of soluble ions of Co(OH)3−. The resultant active sites exhibit reduced maximum energy barriers for the optimized alkaline HER. Additionally, MoO42− near the interface between α‐Co(OH)2 and electrolyte can alleviate the accumulation of hydroxyl ions on α‐Co(OH)2 due to the electrostatic repulsion, improving the stability toward HER. This work offers insight into the role of coordination polyhedron ions in regulating and enhancing the stability of α‐Co(OH)2 for various potential electrochemical applications in alkaline electrolyte.

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The Underlying Molecular Mechanism of Fence Engineering to Break the Activity–Stability Trade‐Off in Catalysts for the Hydrogen Evolution Reaction

Cited by 5 publications

References 55 publications

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

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

A self-healing electrocatalytic system via electrohydrodynamics induced evolution in liquid metal

Boosting the Stability of Oxygen Vacancies in α‐Co(OH)₂ Nanosheets with Coordination Polyhedrons as Rivets for High‐Performance Alkaline Hydrogen Evolution Electrocatalyst

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The Underlying Molecular Mechanism of Fence Engineering to Break the Activity–Stability Trade‐Off in Catalysts for the Hydrogen Evolution Reaction

Cited by 5 publications

References 55 publications

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

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

A self-healing electrocatalytic system via electrohydrodynamics induced evolution in liquid metal

Boosting the Stability of Oxygen Vacancies in α‐Co(OH)2 Nanosheets with Coordination Polyhedrons as Rivets for High‐Performance Alkaline Hydrogen Evolution Electrocatalyst

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Boosting the Stability of Oxygen Vacancies in α‐Co(OH)₂ Nanosheets with Coordination Polyhedrons as Rivets for High‐Performance Alkaline Hydrogen Evolution Electrocatalyst