Unravelling the key factors in the chlorine-promoted epoxidation of ethylene over a silver–copper oxide nanocatalyst

Urbiztondo, M.A.; Ramírez, Adrián; Hueso, José L.; Santamaría, Jesús A.; Ruiz‐Salvador, A. Rabdel; Hamad, Said

doi:10.1039/d2nr00702a

Cited by 6 publications

(4 citation statements)

References 54 publications

(103 reference statements)

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“…Ag‐based catalysts are irreplaceable for the industrial application of ethylene epoxidation [69–73] . Remarkably, the prepared Ag/Al−MnO 2 shows enhanced activity and ethylene oxide (EO) selectivity in the ethylene epoxidation process.…”

Section: Resultsmentioning

confidence: 99%

“…[60,61] Ag-based catalysts are irreplaceable for the industrial application of ethylene epoxidation. [69][70][71][72][73] Remarkably, the prepared Ag/AlÀ MnO 2 shows enhanced activity and ethylene oxide (EO) selectivity in the ethylene epoxidation process. The ethylene conversion using Ag/AlÀ MnO 2 reaches 100 % with high selectivity to EO (~90 %) at 170 °C and atmospheric pressure (Figure 3a,b).…”

Section: Methodsmentioning

confidence: 99%

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Tailoring the Electronic Metal‐Support Interactions in Supported Silver Catalysts through Al modification for Efficient Ethylene Epoxidation

Yang,

Li,

Liu

et al. 2024

Angewandte Chemie

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Metal‐modified catalysts have attracted extraordinary research attention in heterogeneous catalysis due to their enhanced geometric and electronic structures and outstanding catalytic performances. Silver (Ag) possesses necessary active sites for ethylene epoxidation, but the catalyst activity is usually sacrificed to obtain high selectivity towards ethylene oxide (EO). Herein, we report that using Al can help in tailoring the unoccupied 3d state of Ag on the MnO2 support through strong electronic metal‐support interactions (EMSIs), overcoming the activity‐selectivity trade‐off for ethylene epoxidation and resulting in a very high ethylene conversion rate (~100%) with 90% selectivity for EO under mild conditions (170 oC and atmospheric pressure). Structural characterization and theoretical calculations revealed that the EMSIs obtained by the Al modification tailor the unoccupied 3d state of Ag, modulating the adsorption of ethylene (C2H4) and oxygen (O2) and facilitating EO desorption, resulting in high C2H4 conversion. Meanwhile, the increased number of positively charge Ag+ lowers the energy barrier for C2H4(ads) oxidation to produce oxametallacycle (OMC), inducing the unexpectedly high EO selectivity. Such an extraordinary electronic promotion provides new promising pathways for designing advanced metal catalysts with high activity and selectivity in selective oxidation reactions.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Tailoring the Electronic Metal‐Support Interactions in Supported Silver Catalysts through Al modification for Efficient Ethylene Epoxidation

Yang,

Li,

Liu

et al. 2024

Angewandte Chemie

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“…Due to its excellent disinfection and sterilization effects, EO is used in large quantities in medical devices and supplies during the COVID-19 pandemic [8]. The global production of EO reached 20 million metric tons in 2009, and the requirement for EO is estimated to raise its annual production rate by 2% by 2025 [9]. There exist the close link between the risk of EO exposure and sectional occupations, such as doctors, nurses, and industrial workers.…”

Section: Introductionmentioning

confidence: 99%

Association of ethylene oxide with nonalcoholic fatty liver disease among US adults.

Yan,

Pei,

et al. 2024

Preprint

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Background Growing evidence suggest that ethylene oxide (EO) may have deleterious effects on health conditions, but the relationship between EO and adulthood nonalcoholic fatty liver disease (NAFLD) remains vague. Our objective is to evaluate whether EO exposure would influence the prevalence of NAFLD in a nationally cross-sectional study. Materials and methods In this cross-sectional study, We analyzed 2,394 participants from the National Health and Nutrition Examination Survey (NHANES) 2013-2018. Blood concentrations of EO were measured using high-performance liquid chromatography coupled with tandem mass spectrometry. US fatty liver index (USFLI) and FLI were applied to define NAFLD. Logistic regression analysis was adopted to investigate the relationship of Hemoglobin adducts of EO (HbEO) exposure with the prevalence of NAFLD. Mediation analysis was performed to assess the effect of inflammatory biomarkers on the association between HbEO levels and USFLI, FLI, and NAFLD. Results After adjustment for age, gender, race/ethnicity, education, income, smoking, drinking, hypertension, diabetes, and TC, logistic regression analysis showed that HbEO in the highest quartile was negatively associated with the prevalence of NAFLD than those in the lowest quartile (OR: 0.50, 95% CI: 0.33-0.92, P for trend = 0.008 for USFLI and OR: 0.42, 95% CI: 0.29-0.61, P for trend <0.001 for FLI). In addition, inflammation significantly mediated the relationships between HbEO and NAFLD. Conclusions Our study demonstrated that higher EO levels were negatively associated with the prevalence of NAFLD. The underlying mechanisms were required to be identify in the future study.

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“…In one of our most recent publications, 22 authors attempted to explain the role of chlorine in this reaction involving ethylene epoxidation over an Ag−CuO hybrid catalyst by theoretical density functional theory (DFT) calculations. The analysis of the experimental data and calculated reaction and adsorption profiles suggests that the observed selectivity is not determined by a single factor but rather by a combination of factors.…”

Section: ■ Introductionmentioning

confidence: 99%

Deep Learning-Based Energy Mapping of Chlorine Effects in an Epoxidation Reaction Catalyzed by a Silver–Copper Oxide Nanocatalyst

Urbiztondo Castro,

Rodrigo,

Hamad

2023

J. Phys. Chem. C

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Deep learning is poised to revolutionize the field of heterogeneous catalysis. In this study, we harness its potential to predict energy values across a catalyst surface, a task traditionally relegated to computationally intensive density functional theory (DFT). We propose a novel deep learning approach to construct an exhaustive energy map, pinpointing the optimal locations for adsorbed chlorine in the ethylene epoxidation reaction. Leveraging the power of trained neural networks, we achieved a staggering reduction in computational time, cutting down the duration of energy calculations by over 50 million times compared with traditional methods. This groundbreaking integration of artificial intelligence not only accelerates this process but also effectively surpasses the limitations of conventional methods. By highlighting the transformative potential of deep learning in catalysis, this research paves the way for future studies and stands to revolutionize efficiency in the chemical industry, fostering an urgent need to delve deeper into the implications and applications of this technology.

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Unravelling the key factors in the chlorine-promoted epoxidation of ethylene over a silver–copper oxide nanocatalyst

Abstract: Ethylene oxide is one of the most important raw materials in the chemical industry, with an annual production close to 35 million metric tons. Despite its importance, to date no...

Cited by 6 publications

References 54 publications

Tailoring the Electronic Metal‐Support Interactions in Supported Silver Catalysts through Al modification for Efficient Ethylene Epoxidation

Tailoring the Electronic Metal‐Support Interactions in Supported Silver Catalysts through Al modification for Efficient Ethylene Epoxidation

Association of ethylene oxide with nonalcoholic fatty liver disease among US adults.

Deep Learning-Based Energy Mapping of Chlorine Effects in an Epoxidation Reaction Catalyzed by a Silver–Copper Oxide Nanocatalyst

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