Hydrogen oxidation reaction in alkaline media: Relationship between electrocatalysis and electrochemical double-layer structure

Ramaswamy, Nagappan; Ghoshal, Shraboni; Bates, Michael K.; Jia, Qingying; Li, Jingkun; Mukerjee, Sanjeev

doi:10.1016/j.nanoen.2017.07.053

Cited by 98 publications

(102 citation statements)

References 41 publications

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“…The positive effect of the surface pre-oxidation on theNi catalytic activity in HOR was also reported previously[52,63]. This observation might serve as a direct experimental evidence of the bifunctional mechanism of HOR[26,50,[64][65][66][67], when OHad species, pre-chemisorbed on the adjacent active sites, are required in order to remove Had chemisorbed on the free metallic surface of Ni, and to make the hydrogen oxidation reaction proceed.Thus, presumably a certain optimal ratio of Ni(OHad)/Ni(Had) sites is needed to retain the HOR activity of bare Ni electrocatalyst. Therefore, the theoretical estimations of HBE and OHBE, provided inFigure 1, (a)and (b), might shed some light on the understanding of the competitive co-adsorption of H and OH species (see section 2.1).…”

supporting

confidence: 83%

“…Pt, Ir, Rh) show two orders of magnitude lower catalytic activity in HOR in alkaline media compared to acidic one[45,49,56], because in the potential range of hydrogen electrooxidation the surfaces produce negligibly low ratio PGM(Had)/PGM(OHad)? The doping of PGMs by TMs with high affinity to chemisorption of OH species was shown to result in the HOR catalysis promotion[67,70,71]. However, this subject is beyond the scope of this work.HOR polarization curves in the potential range of 0÷0.4 V, presented in Figures 3 (a) and (b), show electrocatalytic behavior of Ni/C, Ni3Fe1/C, Ni3Co1/C and Ni3Cu1/C typical for polycrystallineNi[51], or TM doped Ni electrocatalysts[34].…”

mentioning

confidence: 92%

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Hydrogen Oxidation on Ni-Based Electrocatalysts: The Effect of Metal Doping

Davydova¹,

Zaffran²,

Dhaka³

et al. 2018

Preprint

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Carbon supported nanoparticles of monometallic Ni catalyst and binary Ni-Transition Metal (Ni-TM/C) electrocatalytic composites were synthesized via chemical reduction method, where TM stands for the doping elements Fe, Co, and Cu. The chemical composition, structure and morphology of the Ni-TM/C materials were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffractometry (XRD), transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM) and energy-dispersive X-ray spectroscopy (EDS). The electrochemical properties towards hydrogen oxidation reaction in alkaline medium were studied using the rotating disc electrode and cycling voltammetry methods. A significant role of the TM dopant in the promotion of the hydrogen electrooxidation kinetics of the binary Ni-TM/C materials were revealed. A record-high in exchange current density value of 0.060 mA cm2Ni was measured for Ni3Fe1/C, whereas the monometallic Ni/C counterpart has only shown 0.039 mA cm2Ni. In order to predict the feasibility of the electrocatalysts for hydrogen chemisorption, density functional theory was applied to calculate the hydrogen binding energy and hydroxide binding energy values for bare Ni and Ni3TM1.

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supporting

confidence: 83%

mentioning

confidence: 92%

Hydrogen Oxidation on Ni-Based Electrocatalysts: The Effect of Metal Doping

Davydova¹,

Zaffran²,

Dhaka³

et al. 2018

Preprint

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“…Here the experimentally obtained d-band vacancies (calculated through the ex situ X-ray absorption near-edge structure spectra (XANES) shown in Supplementary Fig. 7) are used to represent the H adsorption ability of the catalysts; the larger vacancy of the Pt’s d-band, the stronger Pt-H bond, and vice versa 36,37 . Afterwards, by quantitatively evaluating the H adsorption ability of a group of different Pt-based nanomaterials, we obtained a relationship between the H adsorption ability and the material’s activity 34 .…”

Section: Resultsmentioning

confidence: 99%

Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions

et al. 2019

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Most fundamental studies of electrocatalysis are based on the experimental and simulation results obtained for bulk model materials. Some of these mechanistic understandings are inapplicable for more active nanostructured electrocatalysts. Herein, considering the simplest and most typical electrocatalytic process, the hydrogen evolution reaction, an alternative reaction mechanism is proposed for nanomaterials based on the identification of a new intermediate, which differs from those commonly known for the bulk counterparts. In-situ Raman spectroscopy and electrochemical thermal/kinetic measurements were conducted on a series of nanomaterials under different conditions. In high-pH electrolytes with negligible hydronium (H3O+) concentration in bulk phase, massive H3O+ intermediates are found generating on the catalytic surface during water dissociation and hydrogen adsorption processes. These H3O+ intermediates create a unique acid-like local reaction environment on nanostructured catalytic surfaces and cut the energy barrier of the overall reaction. Such phenomena on nanostructured electrocatalysts explain their widely observed anomalously high activity under high-pH conditions.

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“…Hydrogen as well as oxygen electrocatalysis will govern electrical performances of the above-mentioned applications. The recent development of anion exchange membranes [2] with useful conductivities in the range of 20-40 mS cm -1 [3] paved the way for the design of solid anion exchange membrane technologies, recently reinforcing the interest to design catalysts evolving in alkaline environments. These media allow using catalysts free from PGM and even free from critical raw materials [4].…”

Section: Introductionmentioning

confidence: 99%

Recent trends in hydrogen and oxygen electrocatalysis for anion exchange membrane technologies

Habrioux

Morais

Napporn

et al. 2020

Current Opinion in Electrochemistry

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HAL is a multi-disciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not. The documents may come from teaching and research institutions in France or abroad, or from public or private research centers. L'archive ouverte pluridisciplinaire HAL, est destinée au dépôt et à la diffusion de documents scientifiques de niveau recherche, publiés ou non, émanant des établissements d'enseignement et de recherche français ou étrangers, des laboratoires publics ou privés.

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Hydrogen oxidation reaction in alkaline media: Relationship between electrocatalysis and electrochemical double-layer structure

Cited by 98 publications

References 41 publications

Hydrogen Oxidation on Ni-Based Electrocatalysts: The Effect of Metal Doping

Hydrogen Oxidation on Ni-Based Electrocatalysts: The Effect of Metal Doping

Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions

Recent trends in hydrogen and oxygen electrocatalysis for anion exchange membrane technologies

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