Platinum overlayers on Pt Ru1−(111) electrodes: Tailoring the ORR activity by lateral strain and ligand effects

Heider, Emanuel; Jacob, Timo; Kibler, Ludwig A.

doi:10.1016/j.jelechem.2017.10.063

Cited by 12 publications

(7 citation statements)

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“…In particular, density functional theory (DFT) has provided deep insight into heterogeneous catalysis as a whole. 7 In situ experimental and computational studies concur that catalytic activities are dictated by the nature of the active sites, which strongly depends on the materials' composition [13][14][15][16][17][18][19][20][21][22] and surface structure, [23][24][25][26] and the electrolyte composition. [27][28][29][30][31] In this perspective, we analyze several fundamental issues related to the elucidation of the electrocatalysts' active centers and factors that modify their catalytic efficiency.…”

Section: Introductionmentioning

confidence: 91%

Revealing the nature of active sites in electrocatalysis

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Section: Introductionmentioning

confidence: 91%

Revealing the nature of active sites in electrocatalysis

et al. 2019

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“…A full monolayer (ML) Ir on Pt(100) thus shows the largest change in binding energies of intermediates (Table ) compared to Pt(100). It is rather difficult to isolate strain, ligand, and ensemble effects in bimetallic PtM catalysts that contain M atom on the surface or in the first or second subsurface layer. − Therefore, both effects are expected to contribute for the observed change in DFT calculated binding energies of the intermediates on PtIr(100) compared to Pt(100) as DFT models of PtIr(100) contain Ir on the surface. According to the Brønsted–Evans–Polanyi (BEP) relationship, the enhanced binding strength of the intermediates should facilitate the C–C bond cleavage.…”

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confidence: 99%

Enhancing C–C Bond Scission for Efficient Ethanol Oxidation using PtIr Nanocube Electrocatalysts

et al. 2019

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Ethanol is a green, sustainable, and high-energy-density liquid fuel that holds great promise for direct liquid fuel cells (DLFCs). However, it remains highly challenging to develop electrocatalysts that selectively promote the C–C bond scission for the ethanol oxidation reaction (EOR). Here, we report the facile synthesis of PtIr alloy core–shell nanocubes (NCs) with Ir-rich shells as effective EOR electrocatalysts. We find that (100)-exposed Pt38Ir NCs with one-atom-thick Ir-rich skin exhibit unprecedented EOR activity, high CO2 selectivity, and long-term stability, while pure Pt NCs and Pt17Ir NCs (two-atom thick Ir-rich skin) show less activity and lower CO2 selectivity. We demonstrate that the Pt38Ir NCs electrocatalyst can deliver a current density up to 4.5 times higher than that of Pt/C with a lower EOR onset potential by 320 mV. Its CO2 current density at 0.85 V is 14 times higher than that of commercial Pt/C. We show that the enhanced EOR activity is mainly due to the Ir-rich PtIr(100) facet that not only favors the splitting of the C–C bond by strongly adsorbing the *C x H y O/C x H y species but also promotes the desorption of CO from the PtIr surface. This work highlights the critical role of surface atom layers on shape-engineered catalysts and demonstrates a strategy for the design of efficient EOR electrocatalysts.

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“…3) Selecting a catalyst carrier with strong interaction with Pt can improve the stability of Pt and Pt‐based catalysts and can also produce a synergistic cocatalytic effect by interaction of Pt nanoparticles with carriers . 4) They can be improved by controlling the shape and crystal plane of the Pt nanocrystals to maximize the exposure of the crystal planes that favor the catalysis of the ORR …”

Section: Introduction To Oxygen Reduction Catalystmentioning

confidence: 99%

Recent Advances and Prospects of Metal‐Based Catalysts for Oxygen Reduction Reaction

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Fuel cells, as one of the most promising technologies in sustainable energy conversion systems, hold great expectations for commercial applications. Cathode oxygen reduction reaction (ORR) kinetics of fuel cells are very slow and require a large overpotential to make the reaction occur, which greatly limits the energy output of fuel cells. Therefore, designing and preparing a highly active and stable ORR catalyst has become a great challenge. Herein, recent advances in platinum‐based and platinum‐free materials in metal‐based catalysts are focused on, including structural properties, synthesis methods, performance characterization, and catalytic mechanisms. Although platinum‐based precious metal catalysts have excellent performance, high prices limit the scale of commercial fuel cells. Nonprecious metal catalysts (e.g., transition metal nitrogen‐doped carbon‐based catalysts (M‐N/C), transition metal compounds (transition metal oxides—TMOs, transition metal carbides—TMCs, transition metal nitrides/transition metal oxynitrides—TMNs/TMNOs), layered double hydroxides—LDHs) completely eliminate dependence on precious metals and exhibit excellent ORR catalytic activity and stability. Finally, the ideas for future design and preparation of new ORR catalysts and challenges in the future of research work are discussed.

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Platinum overlayers on Pt Ru1−(111) electrodes: Tailoring the ORR activity by lateral strain and ligand effects

Cited by 12 publications

References 50 publications

Revealing the nature of active sites in electrocatalysis

Revealing the nature of active sites in electrocatalysis

Enhancing C–C Bond Scission for Efficient Ethanol Oxidation using PtIr Nanocube Electrocatalysts

Recent Advances and Prospects of Metal‐Based Catalysts for Oxygen Reduction Reaction

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