Hydrogen Evolution Reaction-From Single Crystal to Single Atom Catalysts

Gutić, Sanjin J.; Dobrota, Ana S.; Fako, Edvin; Skorodumova, Natalia V.; López, Núria; Pašti, Igor A.

doi:10.3390/catal10030290

Cited by 55 publications

(42 citation statements)

References 196 publications

(233 reference statements)

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“…50 Different from the traditional doping or hybrid, the single atoms with high atomic utilization efficiency could not only largely reduce the usage of heteroatoms, but also will provide a potential solution to verify the detailed function of the heteroatom. 51 Construction of electrochemical heterogeneous interfaces can expose more active sites and produce a more favorable interface to improve catalytic activity. 52,53 For such periodic structure, each unilamellar nanosheet simultaneously acts as both the active component and the interface to maximize to structural advantages from the molecular-scale modulation.…”

Section: Design Strategies For Ni-fe Based Compounds For Electrocatalmentioning

confidence: 99%

Recent progress of Ni–Fe layered double hydroxide and beyond towards electrochemical water splitting

et al. 2020

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Section: Design Strategies For Ni-fe Based Compounds For Electrocatalmentioning

confidence: 99%

Recent progress of Ni–Fe layered double hydroxide and beyond towards electrochemical water splitting

et al. 2020

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“…The mechanism described by eqs. (10)(11)(12) predicts the Tafel slope of 120 mV dec -1 if the first step described by eq. (10) is the rate determining step (rds), 40 mV dec -1 if the second step described by eq.…”

Section: Electrochemical Characterization Of Prepared Electrodes In Pmentioning

confidence: 99%

“…In each specific solution, PtOy, IrO2 and mixed coupled xPtOy-(100-x)IrO2 electrodes studied here, generally follow the same oxygen evolution reaction pathway described by equations (6-9) or (10-13), but with different rate determining steps. Note that OER reaction pathways described by equations (6)(7)(8)(9) and equations (10)(11)(12) are generally known as the oxide decomposition path and the electrochemical oxide path, respectively [43].…”

Section: S + H2o → S-oh* + H + + E -(13a)mentioning

confidence: 99%

“…The overall water splitting reaction includes the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). To realize the practical and sustainable application of electrocatalytic hydrogen/oxygen evolution reactions (HER/OER), an efficient, durable, and economical electrocatalyst is demanded triggering the reaction with minimal overpotential and fast kinetics [9][10][11].…”

Section: Introductionmentioning

confidence: 99%

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Study of oxygen evolution reaction on thermally prepared xPtOy-(100-x)IrO2 electrodes

Ollo¹,

Pohan

Kondro

et al. 2020

J. Electrochem. Sci. Eng.

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The mixed coupled xPtOy-(100-x)IrO2 electrodes (x = 0, 10, 20, 30, 40, 50, 60, 70, 80, 90 and 100) were thermally prepared at 450 °C on titanium supports. The prepared electrodes were firstly physically characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Afterwards, electrochemical characterizations were performed by voltammetric (cyclic and linear) methods in different electrolyte media (KOH and HClO4). It is shown that the prepared electrodes are composed by both PtOy (platinum and platinum oxide) and IrO2 (iridium dioxide). For xPtOy-(100-x)IrO2 electrodes having higher content of IrO2, more surface cracks and pores are formed, defining a higher surface area with more active sites. Higher surface area due to presence of both PtOy and IrO2, is for xPtOy-(100-x)IrO2 electrodes in 1 M KOH solution confirmed by cyclic voltammetry at potentials of the oxide layer region. For all prepared electrodes, voltammetric charges were found higher than for PtOy, while the highest voltammetric charge is observed for the mixed 40PtOy-60IrO2 (x = 40) electrode. The Tafel slopes for oxygen evolution reaction (OER) in either basic (0.1 M KOH) or acid (0.1 M HClO4) media were determined from measured linear voltammograms corrected for the ohmic drop. The values of Tafel slopes for OER at PtOy, 90PtOy-10IrO2 and IrO2 in basic medium are 122, 55 and 40 mV dec-1, respectively. For other mixed electrodes, Tafel slopes of 40 mV dec-1 were obtained. Although proceeding by different OER mechanism, similar values of Tafel slopes were obtained in acid medium, i.e., Tafel slopes of 120, 60 and 39 mV dec-1 were obtained for PtOy, 90PtOy-10IrO2 and IrO2, and 40 mV dec-1 for other mixed electrodes. The analysis of Tafel slope values showed that OER is more rapid on coupled mixed electrodes than on pure PtOy. For mixed xPtOy-(100-x)IrO2 electrodes, OER is more rapid when the molar percent of PtOy meets the following condition: 0 ˂ x ≤ 80. This study also showed that the mixed coupled electrodes are more electrocatalytically active for OER than either PtOy or IrO2 in these two media.

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“…Since virtually every atom possesses catalytic function, even SACs based on Pt-group metals are attractive for practical applications. So far, the use of SACs has been demonstrated for numerous catalytic and electrocatalytic reactions, including energy conversion and storage-related processes such as hydrogen evolution reactions (HER) [4][5][6][7][8][9], oxygen reduction reactions (ORR) [7,[10][11][12], oxygen evolution reactions (OER) [8,13,14], and others. Moreover, SACs can be modeled relatively easily, as the single-atom nature of active sites enables the use of small computational models that can be treated without any difficulties.…”

Section: Introductionmentioning

confidence: 99%

What Is the Real State of Single-Atom Catalysts under Electrochemical Conditions—From Adsorption to Surface Pourbaix Plots?

et al. 2021

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The interest in single-atom catalysts (SACs) is increasing, as these materials have the ultimate level of catalyst utilization, while novel reactions where SACs are used are constantly being discovered. However, to properly understand SACs and to further improve these materials, it is necessary to consider the nature of active sites under operating conditions. This is particularly important when SACs are used as electrocatalysts due to harsh experimental conditions, including extreme pH values or high anodic and cathodic potential. In this contribution, density functional theory-based thermodynamic modelling is used to address the nature of metal centers in SACs formed by embedding single metal atoms (Ru, Rh, Ir, Ni, Pd, Pt, Cu, Ag, and Au) into graphene monovacancy. Our results suggest that none of these SAC metal centers are clean at any potential or pH in the water thermodynamic stability region. Instead, metal centers are covered with Hads, OHads, or Oads, and in some cases, we observed the restructuring of the metal sites due to oxygen incorporation. Based on these findings, it is suggested that setting up theoretical models for SAC modelling and the interpretation of ex situ characterization results using ultra-high vacuum (UHV) techniques requires special care, as the nature of SAC active sites under operating conditions can significantly diverge from the basic models or the pictures set by the UHV measurements.

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Hydrogen Evolution Reaction-From Single Crystal to Single Atom Catalysts

Cited by 55 publications

References 196 publications

Recent progress of Ni–Fe layered double hydroxide and beyond towards electrochemical water splitting

Recent progress of Ni–Fe layered double hydroxide and beyond towards electrochemical water splitting

Study of oxygen evolution reaction on thermally prepared xPtOy-(100-x)IrO2 electrodes

What Is the Real State of Single-Atom Catalysts under Electrochemical Conditions—From Adsorption to Surface Pourbaix Plots?

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