Why the activity of the hydrogen oxidation reaction on platinum decreases as pH increases

Briega-Martos, Valentín; Ferre-Vilaplana, Adolfo; Herrero, Enrique; Feliú, Juan M.

doi:10.1016/j.electacta.2020.136620

Cited by 35 publications

(44 citation statements)

References 78 publications

(133 reference statements)

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“…5a and Supplementary Fig. 7a), since only the wave related to the H 2 oxidation was observed at the Pt ring 69 . The current associated with this process is higher in the phosphate buffer solution, suggesting that the production of hydrogen is favoured in this media.…”

Section: Co2rr Activity and Products Analysismentioning

confidence: 99%

Copper single-atoms embedded in 2D graphitic carbon nitride for the CO2 reduction

et al. 2021

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We report the study of two-dimensional graphitic carbon nitride (GCN) functionalized with copper single atoms as a catalyst for the reduction of CO2 (CO2RR). The correct GCN structure, as well as the adsorption sites and the coordination of the Cu atoms, was carefully determined by combining experimental techniques, such as X-ray diffraction, transmission electron microscopy, X-ray absorption, and X-ray photoemission spectroscopy, with DFT theoretical calculations. The CO2RR products in KHCO3 and phosphate buffer solutions were determined by rotating ring disk electrode measurements and confirmed by 1H-NMR and gas chromatography. Formate was the only liquid product obtained in bicarbonate solution, whereas only hydrogen was obtained in phosphate solution. Finally, we demonstrated that GCN is a promising substrate able to stabilize metal atoms, since the characterization of the Cu-GCN system after the electrochemical work did not show the aggregation of the copper atoms.

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Section: Co2rr Activity and Products Analysismentioning

confidence: 99%

Copper single-atoms embedded in 2D graphitic carbon nitride for the CO2 reduction

et al. 2021

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“…Moreover, the H ad on the electrode surface is the key intermediate of hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR), and its adsorption energy is widely used as a descriptor for the reaction activity. 32 − 36 In view of these interests, many efforts have been devoted to modeling the Pt(111)-H ad /water interfaces in recent years. 37 − 40 For example, Kristoffersen et al 39 have shown that the H ad atoms are mostly distributed on the hollow and top sites on Pt(111) and effectively replace the chemisorbed water on the surface.…”

Section: Introductionmentioning

confidence: 99%

Modeling Electrified Pt(111)-H_ad/Water Interfaces from Ab Initio Molecular Dynamics

Chen

et al. 2021

JACS Au

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Unraveling the atomistic structures of electric double layers (EDL) at electrified interfaces is of paramount importance for understanding the mechanisms of electrocatalytic reactions and rationally designing electrode materials with better performance. Despite numerous efforts dedicated in the past, a molecular level understanding of the EDL is still lacking. Combining the state-of-the-art ab initio molecular dynamics (AIMD) and recently developed computational standard hydrogen electrode (cSHE) method, it is possible to realistically simulate the EDL under well-defined electrochemical conditions. In this work, we report extensive AIMD calculation of the electrified Pt(111)-H ad /water interfaces at the saturation coverage of adsorbed hydrogen (H ad ) corresponding to the typical hydrogen evolution reaction conditions. We calculate the electrode potentials of a series of EDL models with various surface charge densities using the cSHE method and further obtain the Helmholtz capacitance that agrees with experiment. Furthermore, the AIMD simulations allow for detailed structural analyses of the electrified interfaces, such as the distribution of adsorbate H ad and the structures of interface water and counterions, which can in turn explain the computed dielectric property of interface water. Our calculation provides valuable molecular insight into the electrified interfaces and a solid basis for understanding a variety of electrochemical processes occurring inside the EDL.

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“…4 for the HPRR are higher than those for the ORR reported in [7]. Additionally, ORR observed here has to be related to the first step in the reaction, that involving the first electron transfer to form the adsorbed OOH is [9,10] or the superoxide anion radical (O 2 ÁÀ ) in alkaline media [11][12][13], since the HPRR is faster than the ORR. On the other hand, the currents in the region where the inhibition takes place show significant differences (Fig.…”

Section: Mechanistic Insights For the Orr Before And After The Formation Of H 2 Omentioning

confidence: 55%

“…) has been postulated for the ORR after the first electron transfer in alkaline media [11][12][13]. Additionally, since H 2 O 2 has been detected as an intermediate in the reaction, the studies of the hydrogen peroxide reduction reaction (HPRR) are also important to elucidate the mechanism of the ORR.…”

Section: áàmentioning

confidence: 99%

New insights into the hydrogen peroxide reduction reaction and its comparison with the oxygen reduction reaction in alkaline media on well-defined platinum surfaces

Rizo

Feliú

Herrero

2021

Journal of Catalysis

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Why the activity of the hydrogen oxidation reaction on platinum decreases as pH increases

Cited by 35 publications

References 78 publications

Copper single-atoms embedded in 2D graphitic carbon nitride for the CO2 reduction

Copper single-atoms embedded in 2D graphitic carbon nitride for the CO2 reduction

Modeling Electrified Pt(111)-H_ad/Water Interfaces from Ab Initio Molecular Dynamics

New insights into the hydrogen peroxide reduction reaction and its comparison with the oxygen reduction reaction in alkaline media on well-defined platinum surfaces

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Why the activity of the hydrogen oxidation reaction on platinum decreases as pH increases

Cited by 35 publications

References 78 publications

Copper single-atoms embedded in 2D graphitic carbon nitride for the CO2 reduction

Copper single-atoms embedded in 2D graphitic carbon nitride for the CO2 reduction

Modeling Electrified Pt(111)-Had/Water Interfaces from Ab Initio Molecular Dynamics

New insights into the hydrogen peroxide reduction reaction and its comparison with the oxygen reduction reaction in alkaline media on well-defined platinum surfaces

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Modeling Electrified Pt(111)-H_ad/Water Interfaces from Ab Initio Molecular Dynamics