CoFe-Layered Double Hydroxide Coupled with Pd Particles for Electrocatalytic Ethanol Oxidation

Song, Weijie; Xu, Yanqi; Xie, Xingyu; Li, Cunjun; Wang, Zhu; Qin, Xiang; Chen, Wei; Tang, Ningli; Wang, Linjiang

doi:10.1021/acsami.3c01541

“…XAFS results confirm the successful formation of the PdÀ OÀ Gd bridge in PdÀ Gd 2 O 3 /C owing to strong interface interaction between Pd and Gd 2 O 3 . [51,52] The formation of the PdÀ OÀ Gd bridge between Pd nanoparticles and Gd 2 O 3 /C can guarantee adequate surface-active site exposure and structural stability.…”

Section: Angewandte Chemiementioning

confidence: 99%

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Ning,

Li,

Wang

et al. 2023

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The active‐site density, intrinsic activity, and durability of Pd‐based materials for oxygen reduction reaction (ORR) are critical to their application in industrial energy devices. This work constructs a series of carbon‐based rare‐earth (RE) oxides (Gd2O3, Sm2O3, Eu2O3, and CeO2) by using RE metal‐organic frameworks to tune the ORR performance of the Pd sites through the Pd‐RExOy interface interaction. Taking Pd‐Gd2O3/C as a representative, it is identified that the strong coupling between Pd and Gd2O3 induces the formation of the Pd‐O‐Gd bridge, which triggers charge redistribution of Pd and Gd2O3. The screened Pd‐Gd2O3/C exhibits impressive ORR performance with high onset potential (0.986 VRHE), half‐wave potential (0.877 VRHE), and excellent stability. Similar ORR results are also found for Pd‐Sm2O3/C, Pd‐Eu2O3/C, and Pd‐CeO2/C catalysts. Theoretical analyses reveal that the coupling between Pd and Gd2O3 promotes electron transfer through the Pd‐O‐Gd bridge, which induces the antibonding‐orbital occupancy of Pd‐*OH for the optimization of *OH adsorption in the rate‐determining step of ORR. The pH‐dependent microkinetic modeling shows that Pd‐Gd2O3 is close to the theoretical optimal activity for ORR, outperforming Pt under the same conditions. By its ascendancy in ORR, the Pd‐Gd2O3/C exhibits superior performance in Zn‐air battery as an air cathode, implying its excellent practicability.

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“…XAFS results confirm the successful formation of the PdÀ OÀ Gd bridge in PdÀ Gd 2 O 3 /C owing to strong interface interaction between Pd and Gd 2 O 3 . [51,52] The formation of the PdÀ OÀ Gd bridge between Pd nanoparticles and Gd 2 O 3 /C can guarantee adequate surface-active site exposure and structural stability.…”

Section: Forschungsartikelmentioning

confidence: 99%

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Ning,

Li,

Wang

et al. 2023

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The active‐site density, intrinsic activity, and durability of Pd‐based materials for oxygen reduction reaction (ORR) are critical to their application in industrial energy devices. This work constructs a series of carbon‐based rare‐earth (RE) oxides (Gd2O3, Sm2O3, Eu2O3, and CeO2) by using RE metal‐organic frameworks to tune the ORR performance of the Pd sites through the Pd‐RExOy interface interaction. Taking Pd‐Gd2O3/C as a representative, it is identified that the strong coupling between Pd and Gd2O3 induces the formation of the Pd‐O‐Gd bridge, which triggers charge redistribution of Pd and Gd2O3. The screened Pd‐Gd2O3/C exhibits impressive ORR performance with high onset potential (0.986 VRHE), half‐wave potential (0.877 VRHE), and excellent stability. Similar ORR results are also found for Pd‐Sm2O3/C, Pd‐Eu2O3/C, and Pd‐CeO2/C catalysts. Theoretical analyses reveal that the coupling between Pd and Gd2O3 promotes electron transfer through the Pd‐O‐Gd bridge, which induces the antibonding‐orbital occupancy of Pd‐*OH for the optimization of *OH adsorption in the rate‐determining step of ORR. The pH‐dependent microkinetic modeling shows that Pd‐Gd2O3 is close to the theoretical optimal activity for ORR, outperforming Pt under the same conditions. By its ascendancy in ORR, the Pd‐Gd2O3/C exhibits superior performance in Zn‐air battery as an air cathode, implying its excellent practicability.

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“…The latest academic research has achieved considerable progress in the field of palladium-based catalysts for improving activity, stability, and selectivity in EOR electrocatalysis, including alloying Pd with foreign elements, heteroatoms doping, crystal structure engineering, and the construction of complex composite nanostructures. − In particular, the decoration of oxygenophilic metal or oxide components onto the surface of Pd nanostructures to construct nanocomposites or heterostructures has risen as an efficacious strategy for optimizing the electrocatalytic properties of Pd, attributed to the synergistic effect of heteroatoms or interfacial effects of these composite systems. For instance, Zhao and co-workers fabricated an array of metal/oxide composites, which encompass transition metal oxides such as Fe, Co, Ni, Cu, and Mn being supported by Pt, Pd, and Ag, along with their inverted systems.…”

Section: Introductionmentioning

confidence: 99%

Ultrafine IrMnO_x Nanocluster Decorated Amorphous PdS Nanowires as Efficient Electrocatalysts for High C1 Selectivity in the Alkaline Ethanol Oxidation Reaction

Ju,

Chen,

Xie

et al. 2024

ACS Appl. Mater. Interfaces

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As a novel electrochemical energy conversion device, direct ethanol fuel cells are currently encountering two significant challenges: CO poisoning and the difficulty of C−C bond cleavage in ethanol. In this work, an amorphous PdS nanowires/ultrafine IrMnO x bimetallic oxides (denoted as a-PdS/IrMnO x NWs) catalyst with abundant oxide/metal (crystalline/ amorphous) inverse heterogeneous interfaces was synthesized via a hydrothermal process succeeded by a nonthermal air-plasma treatment. This unique interfacial electronic structure along with the incorporation of oxyphilic metal has resulted in a significant enhancement in the electrocatalytic performance of a-PdS/IrMnO x NWs toward the ethanol oxidation reaction, achieving current densities of 12.45 mA•cm −2 and 3.68 A•mg Pd −1 . Moreover, the C1 pathway selectivity for ethanol oxidation has been elevated to 47%, exceeding that of other as-prepared Pd-based counterparts and commercial Pd/C catalysts. Density functional theory calculations have validated the findings that the decoration of IrMn species onto the amorphous PdS surface has induced a charge redistribution in the interface region. The redistribution of surface charges on the a-PdS/IrMnO x NWs catalyst results in a significant decrease in the activation energy required for C−C bond cleavage and a notable weakening of the CO binding strength at the Pd active sites. Consequently, it enhanced both the EOR C1 pathway selectivity and CO poisoning resistance to the a-PdS/IrMnO x NWs catalyst.

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CoFe-Layered Double Hydroxide Coupled with Pd Particles for Electrocatalytic Ethanol Oxidation

Cited by 9 publications

References 58 publications

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Ultrafine IrMnO_x Nanocluster Decorated Amorphous PdS Nanowires as Efficient Electrocatalysts for High C1 Selectivity in the Alkaline Ethanol Oxidation Reaction

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CoFe-Layered Double Hydroxide Coupled with Pd Particles for Electrocatalytic Ethanol Oxidation

Cited by 9 publications

References 58 publications

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Ultrafine IrMnOx Nanocluster Decorated Amorphous PdS Nanowires as Efficient Electrocatalysts for High C1 Selectivity in the Alkaline Ethanol Oxidation Reaction

Contact Info

Product

Resources

About

Ultrafine IrMnO_x Nanocluster Decorated Amorphous PdS Nanowires as Efficient Electrocatalysts for High C1 Selectivity in the Alkaline Ethanol Oxidation Reaction