Engineering the Electronic Structure of Submonolayer Pt on Intermetallic Pd<sub>3</sub>Pb via Charge Transfer Boosts the Hydrogen Evolution Reaction

Yao, Yancai; Gu, Xiang-Kui; He, Dongsheng; Li, Zhijun; Liu, Wei; Xu, Qian; Yao, Takeshi; Lin, Yue; Wang, Huijuan; Zhao, Changming; Wang, Xiaoqian; Yin, Peiqun; Li, Hai; Hong, Xun; Wei, Shiqiang; Li, Wei‐Xue; Li, Yadong; Wu, Yuen

doi:10.1021/jacs.9b09391

Cited by 110 publications

(66 citation statements)

References 32 publications

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“…1f, the atomic resolution high-angle annular dark field-scanning TEM (HAADF-STEM) image displays a periodic light and dark contrast arrangement. As reported, the atomic number determines the brightness of an atom column in an HAADF-STEM image [23]; thus the brightness level of atoms is Ir (77) > Pr (59). Energy dispersive spectroscopy (EDS) mapping ( Fig.…”

Section: +mentioning

confidence: 79%

Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

et al. 2021

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Amorphous iridium oxides (IrO x) are highly active for oxygen evolution reaction (OER) in acid media; however, it is generally unstable compared with commercial IrO 2. Recently, many non-noble metal-iridium mixed oxides are prepared for catalyzing OER efficiently. Herein, we report a cubic fluorite-type praseodymium iridium oxide with the surface of IrO x (IrO x /Pr 3 IrO 7) that shows the improved activity and stability in 0.1 mol L −1 HClO 4 solution, characterized by an overpotential of 305 mV at the benchmark of 10 mA cm −2 and a small Tafel slope of 37 mV dec −1 , indicating a fast reaction kinetics and a competitive activity compared with the benchmark IrO 2 and most reported electrocatalysts. The initial potential increases by less than 0.07 V after continuous OER testing over 60,000 s. In contrast, IrO 2 becomes nearly inactive for the OER within 20,000 s. Density functional theory calculations uncover that the optimal energy level path follows lattice oxygen mechanism (LOM). This work enlarges the family of the IrO x-type OER electrocatalyst in acid media.

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Section: +mentioning

confidence: 79%

Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

et al. 2021

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“…[26,27] In addition, the XPS features of Rh 3d are shifted to lower binding energy (≈0.4 eV) compared with that of Rh nanoparticles, indicative of electron transfer from the PtBi and PtBi@ Pt matrix to Rh atoms in the PtBi-3.6% Rh 1 and PtBi@PtRh 1 nanoplates, respectively (Figure 2d; Figure S25, the Supporting Information). [43] As shown in Figure S26 in the Supporting Information, PtBi@Pt nanoplates were synthesized as well for comparison, by electrochemical dealloying of PtBi intermetallic nanoplates.…”

Section: Resultsmentioning

confidence: 99%

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

et al. 2021

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which is also considered a biorenew able energy carrier. However, the anodic ethanol oxidation reaction (EOR) is a complicated and kinetically sluggish process, involving the transfer of multiple electrons and various reaction intermediates and products. Typically, the C2-pathway dominates the EOR in both acidic and alkaline electrolytes, resulting in the formation of acetic acid or acetate by delivering four electrons, and acetaldehyde by delivering two electrons, respectively. The C1-pathway, which involves complete oxidation and the transfer of 12 electrons generating CO 2 or carbonate, is preferred to the C2-pathway, aiming for maximum DEFCs efficiency. [1][2][3][4][5] Specially, highly efficient catalysts have been developed by engineering Pt-based nanocrystals, and the C1-pathway selectivity has been promoted by Rh-based catalysts. [6][7][8][9] In designing electrochemical surfaces toward maximum performance, modifying the electronic structure and strain of catalytic surfaces are considered state-of-the-art strategies, which can for instance be achieved by introducing metals with different intrinsic reactivities and constructing core-shell nanostructures, respectively. [10][11][12][13][14][15] Combining these approaches in a rational manner would be a promising way to substantially improve the EOR, yet the underlying knowledge about their contributions is largely lacking. [10][11][12][13][14][15][16][17][18] Therefore, it is highly desirable to employ tailored nanostructures to resolve these important issues and contribute to the practical deployment of DEFCs by identifying versatile EOR electrocatalysts possessing high atom utilization of noble metals, high mass-normalized activity at low overpotentials, high C1-pathway selectivity, long-term durability, and superior anti-poisoning ability. [1] To maximize atom utilization, single-atom catalysts (SACs) have emerged as one of the most promising frontiers in materials chemistry. [19][20][21] Using specific support materials such as reducible metal oxides, activated carbons, and anisotropic materials such as MoS 2 , single atoms of catalytically metals can be stabilized, which exhibit intriguing physicochemical properties compared with their counterpart clusters and nanoparticles. [22][23][24] Typically, high-performance EOR catalysts should facilitate multiple dehydrogenation and oxidation steps as well as CC bond cleavage reactions. All these reactions typically require ensembles of surface metal atoms, implying that thisThe rational design and control of electrocatalysts at single-atomic sites could enable unprecedented atomic utilization and catalytic properties, yet it remains challenging in multimetallic alloys. Herein, the first example of isolated Rh atoms on ordered PtBi nanoplates (PtBi-Rh 1 ) by atomic galvanic replacement, and their subsequent transformation into a tensile-strained Pt-Rh single-atom alloy (PtBi@PtRh 1 ) via electrochemical dealloying are presented. Benefiting from the Rh 1 -tailored Pt (110) surface with tensile strain, the PtBi@...

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“…The state-of-the-art catalyst is noble metal catalyst, especially Pt-based catalyst. [104,105] Therefore, research on non-noble metal-based catalysts has become a hot topic, for example, some cheap transition metals and their derivatives. [106][107][108][109] The HER process follows Volmer-Heyrovsky mechanism (Tafel slope: 40~120 mV • dec À 1 ) or Volmer-Tafel mechanism (Tafel slope: 0~40 mV • dec À 1 ).…”

Section: Application Of Ceo 2 -Based Electrocatalysts In Hermentioning

confidence: 99%

“…Hydrogen evolution reaction is one of the core reactions of water electrolysis. The state‐of‐the‐art catalyst is noble metal catalyst, especially Pt‐based catalyst [104,105] . Therefore, research on non‐noble metal‐based catalysts has become a hot topic, for example, some cheap transition metals and their derivatives [106–109] .…”

Section: Application Of Ceo2‐based Electrocatalysts In Hermentioning

confidence: 99%

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

2021

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wards the oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and nitrogen reduction reaction (NRR) are summarized. This Review also highlights the key role of CeO 2 and the structural design strategies in the hybrid electrocatalysts, including ion doping, interface and defect engineering, electronic structure optimization, and morphology control for catalytic output enhancement. Lastly, some scientific challenges and perspectives have been proposed, aiming to promote the development of other CeO 2-based hybrids for energy related electrocatalysis.

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Engineering the Electronic Structure of Submonolayer Pt on Intermetallic Pd₃Pb via Charge Transfer Boosts the Hydrogen Evolution Reaction

Cited by 110 publications

References 32 publications

Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

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Engineering the Electronic Structure of Submonolayer Pt on Intermetallic Pd3Pb via Charge Transfer Boosts the Hydrogen Evolution Reaction

Cited by 110 publications

References 32 publications

Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

Recent Advances of CeO2‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

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Engineering the Electronic Structure of Submonolayer Pt on Intermetallic Pd₃Pb via Charge Transfer Boosts the Hydrogen Evolution Reaction

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction