Vibration-driven reaction of CO2 on Cu surfaces via Eley–Rideal-type mechanism

Quan, Jiamei; Muttaqien, Fahdzi; Kondo, Takahiro; Kozarashi, Taijun; Mogi, Tomoyasu; Imabayashi, Takumi; Hamamoto, Yoshisuke; Inagaki, Kouji; Hamada, Ikutaro; Morikawa, Yoshitada; Nakamura, Junji

doi:10.1038/s41557-019-0282-1

Cited by 82 publications

(82 citation statements)

References 53 publications

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“…Most of the theoretical studies on the competition of electrochemical N 2 reduction and HER are discussed based on E‐R mechanism and Volmer‐Heyrovsky mechanism, respectively [67,84,85] . However, the binding energies of hydrogen atom on the studied catalyst surfaces are generally strong.…”

Section: Resultsmentioning

confidence: 99%

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

Shi

Xiang

et al. 2021

ChemSusChem

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Electrochemical reduction of nitrogen to produce ammonia at moderate conditions in aqueous solutions holds great prospect but also faces huge challenges. Considering the high selectivity of Au‐based materials to inhibit competitive hydrogen evolution reaction (HER) and high activity of transition metals such as Fe and Mo toward the nitrogen reduction reaction (NRR), it was proposed that Au‐based alloy materials could act as efficient catalysts for N2 fixation based on density functional theory simulations. Only on Mo3Au(111) surface the adsorption of N2 is stronger than H atom. Thermodynamics combined with kinetics studies were performed to investigate the influence of composition and ratio of Au‐based alloys on NRR and HER. The binding energy and reorganization energy affected performance for the initial N2 activation and hydrogenation process. By considering the free‐energy diagram, the computed potential‐determining step was either the first or the fifth hydrogenation step on metal catalysts. The optimum catalytic activity could be achieved by adjusting atomic proportion in alloys to make all intermediate species exhibit moderate adsorption. Free‐energy diagrams of N2 hydrogenation via Langmuir‐Hinshelwood mechanism and hydrogen evolution via Tafel mechanism were compared to reveal that the Mo3Au surface showed satisfactory catalytic performance by simultaneously promoting NRR and suppressing HER. Theoretical simulations demonstrated that Au‐Mo alloy materials could be applied as high‐performance electrocatalysts for NRR.

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Section: Resultsmentioning

confidence: 99%

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

Shi

Xiang

et al. 2021

ChemSusChem

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“…96,244 A recent study also showed that vibrational excitation could enhance Eley-Rideal reactions of molecular species. 245 Such reactions are typically negligible under thermal conditions and it is not fully understood to what extent they contribute to the total conversion under plasma conditions. These mechanisms and how they impact the total conversion and energy efficiency will be discussed in more detail in section 5.3.…”

Section: Green Chemistrymentioning

confidence: 99%

Plasma-driven catalysis: green ammonia synthesis with intermittent electricity

et al. 2020

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“…49 However, for copper, there is strong experimental evidence that formate formation proceeds via the Eley-Rideal pathway, in which only hydrogen is chemisorbed at the surface, and CO 2 reacts from the gas phase or physisorbed state. 50 A crucial difference between the processes 2 and 3 is the additional hydrogen containing intermediate (formate) that is formed during the associative pathway. In both reactions, water is formed and its reaction from OH * and H* is slow 38 and thus reduces the overall reaction yield.…”

Section: Excess Hydrogen During Catalysismentioning

confidence: 99%