Production of Acetaldehyde via Oxidative Dehydrogenation of Ethanol over AgLi/SiO2 Catalysts

Mukda, Narawich; Autthanit, Chaowat; Praserthdam, Piyasan; Jongsomjit, Bunjerd

doi:10.9767/bcrec.15.3.8702.714-725

Cited by 2 publications

(1 citation statement)

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“…We note that further combustion of AA on AgO x surfaces leads to the CO 2 byproduct . The ease of AA combustion on Ag surfaces is well established, − and therefore, we did not study it in this work. Alternatively, gas-phase ethylene can react with dissociated atomic oxygen species, forming EO directly via an ER mechanism.…”

Section: Resultsmentioning

confidence: 99%

Mechanisms of Ethylene Epoxidation over Silver from Machine Learning-Accelerated First-Principles Modeling and Microkinetic Simulations

Liu

Ann

et al. 2023

ACS Catal.

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We employed machine learning-augmented density functional theory (DFT) thermodynamic calculations to assess the stability of different AgO x structures under catalytic ethylene epoxidation reaction conditions. We found that there are multiple AgO x surface motifs that could co-exist under the relevant conditions. These included Ag surface oxides (e.g., AgO_p(4 × 4) and Ag 1.83 O) and atomic oxygen-covered Ag(111) surfaces. Furthermore, we employed DFT calculations to evaluate the energetics of different reaction mechanisms by which ethylene and oxygen can react on these surfaces. These studies revealed several energetically viable reaction pathways for ethylene epoxidation. Microkinetic modeling analyses, based on the DFT-calculated reaction pathways, showed that ethylene epoxidation can proceed on all surfaces and that multiple pathways, including those involving Langmuir−Hinshelwood and Eley−Rideal mechanisms, could be involved in selective and unselective reactions. The diversity of mechanisms that we discovered in the context of the relatively simple ethylene epoxidation reaction on Ag suggests that the richness and complexity of surface chemistry are most likely a rule rather than an exception in heterogeneous catalytic chemical transformations on metal surfaces and that the concept of a single or even a dominant mechanism and reaction intermediates might need to be revisited for many reactions.

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