Pt nanostructures with different Rh surface entities: Impact on NH3 electro-oxidation

Fomena, Nadège Nzone; Garbarino, Sébastien; Bertin, Erwan; Korinek, Andreas; Botton, Gianluigi A.; Roué, Lionel; Guay, Daniel

doi:10.1016/j.jcat.2017.08.026

Journal of Catalysis

2017

DOI: 10.1016/j.jcat.2017.08.026

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Pt nanostructures with different Rh surface entities: Impact on NH3 electro-oxidation

Nadège Nzone Fomena

Sébastien Garbarino

Erwan Bertin

et al.

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Cited by 13 publications

(2 citation statements)

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“…Rhodium (Rh) is a promising catalyst for many reactions, including hydrogenation reactions, , ammonia oxidation, nitrite reduction, etc. Recently, Rh was identified as a possible electrode material for electrochemical nitrogen reduction reaction (NRR). − Herein, we have performed a joint experimental and theoretical investigation of N 2 activation on Rh n + clusters by making good use of the plasma effect to molecular beam technique.…”

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confidence: 99%

“…42,43 However, it is still challenging to observe a direct reaction product with an odd number of nitrogen atoms in mild conditions, and the insights of metal cluster catalysis for N≡N bond dissociation are open to be further explored. Rhodium (Rh) is a promising catalyst for many reactions, including hydrogenation reactions, 44,45 ammonia oxidation, 46 nitrite reduction, 47 etc. Recently, Rh was identified as a possible electrode material for electrochemical nitrogen reduction reaction (NRR).…”

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confidence: 99%

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Plasma-Assisted Chain Reactions of Rh₃⁺ Clusters with Dinitrogen: N≡N Bond Dissociation

Cui

Jia

Zhang

et al. 2020

J. Phys. Chem. Lett.

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Dinitrogen activation is known as one of the most challenging subjects in chemistry. A number of well-defined metal complexes, nitrides, and clusters have been studied that show catalysis for dinitrogen activation. However, direct evidence of a complete cleavage of the N≡N triple bond at mild conditions is rather limited to date. Herein, we report a study on the dissociation of N2 on small rhodium clusters assisted by surface plasma radiation. From mass spectrometry observation, a few rhodium nitride clusters with an odd number of nitrogen atoms are produced, such as the Rh3N2m–1 + (m = 1–5) series, indicative of N≡N bond dissociation in the mild plasma atmosphere. Interestingly, Rh3N7 + is identified with outstanding mass abundance among the Rh n N2m–1 + products, and its ground-state structure is in the form of Rh3N(N2)3 + by capping a nitrogen atom on the top of Rh3 + plane and hanging three N2 molecules beneath the three Rh atoms respectively, giving rise to a C 3v symmetry and excellent stability. We demonstrate the catalysis of such a three-atom rhodium cluster and reveal a dinitrogen activation strategy by thermodynamics- and dynamics- favorable chain reactions of multiple N2 molecules with two rhodium clusters under plasma atmosphere.

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mentioning

confidence: 99%

mentioning

confidence: 99%

Plasma-Assisted Chain Reactions of Rh₃⁺ Clusters with Dinitrogen: N≡N Bond Dissociation

Cui

Jia

Zhang

et al. 2020

J. Phys. Chem. Lett.

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Emerging Materials and Methods toward Ammonia‐Based Energy Storage and Conversion

et al. 2021

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Efficient storage and conversion of renewable energies is of critical importance to the sustainable growth of human society. With its distinguishing features of high hydrogen content, high energy density, facile storage/transportation, and zero-carbon emission, ammonia has been recently considered as a promising energy carrier for long-term and large-scale energy storage. Under this scenario, the synthesis, storage, and utilization of ammonia are key components for the implementation of ammonia-mediated energy system. Being different from fossil fuels, renewable energies normally have intermittent and variable nature, and thus pose demands on the improvement of existing technologies and simultaneously the development of alternative methods and materials for ammonia synthesis and storage. The energy release from ammonia in an efficient manner, on the other hand, is vital to achieve a sustainable energy supply and complete the nitrogen circle. Herein, recent advances in the thermal-, electro-, plasma-, and photocatalytic ammonia synthesis, ammonia storage or separation, ammonia thermal/ electrochemical decomposition and conversion are summarized with the emphasis on the latest developments of new methods and materials (catalysts, electrodes, and sorbents) for these processes. The challenges and potential solutions are discussed.

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Promotion of Glycerol Oxidation by Selective Ru Decoration of (100) Domains at Nanostructured Pt Electrodes

et al. 2019

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Glycerol (GlOH) electrooxidation is a potential route to GlOH valorisation. In this work, we show that GlOH oxidation can be enhanced at bimetallic PtÀ Ru electrodes with respect to bare Pt in sulphuric acid. We electrodeposited high-surface area Pt electrodes comprising of 40 % (100) sites, along with a smaller amount of (111) domains. Spontaneous Ru deposition was carried out by immersion in a RuCl 3 solution for a varying amount of time. Voltammetric methods demonstrated that (100) sites are decorated most readily. PtÀ Ru electrodes display an earlier onset potential for CO ads oxidation, which translates into an anticipation of the main GlOH oxidation wave. Under prolonged Ru deposition, Ru decoration also proceeds close to (111) Pt domains, as highlighted by CO stripping. We suggest that such ensembles may play a critical role in achieving optimal GlOH activity at PtÀ Ru.

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Pt nanostructures with different Rh surface entities: Impact on NH3 electro-oxidation

Cited by 13 publications

References 61 publications

Plasma-Assisted Chain Reactions of Rh₃⁺ Clusters with Dinitrogen: N≡N Bond Dissociation

Plasma-Assisted Chain Reactions of Rh₃⁺ Clusters with Dinitrogen: N≡N Bond Dissociation

Emerging Materials and Methods toward Ammonia‐Based Energy Storage and Conversion

Promotion of Glycerol Oxidation by Selective Ru Decoration of (100) Domains at Nanostructured Pt Electrodes

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Product

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Pt nanostructures with different Rh surface entities: Impact on NH3 electro-oxidation

Cited by 13 publications

References 61 publications

Plasma-Assisted Chain Reactions of Rh3+ Clusters with Dinitrogen: N≡N Bond Dissociation

Plasma-Assisted Chain Reactions of Rh3+ Clusters with Dinitrogen: N≡N Bond Dissociation

Emerging Materials and Methods toward Ammonia‐Based Energy Storage and Conversion

Promotion of Glycerol Oxidation by Selective Ru Decoration of (100) Domains at Nanostructured Pt Electrodes

Contact Info

Product

Resources

About

Plasma-Assisted Chain Reactions of Rh₃⁺ Clusters with Dinitrogen: N≡N Bond Dissociation

Plasma-Assisted Chain Reactions of Rh₃⁺ Clusters with Dinitrogen: N≡N Bond Dissociation