Enhanced methanol production over non-promoted Cu-MgO-Al2O3 materials with ex-solved 2 nm Cu particles: Insights from an Operando spectroscopic study Article Swipe
Jorge Cored
,
Jaime Mazarío
,
Cristina Cerdá-Moreno
,
Pablo G. Lustemberg
,
M. V. Ganduglia-Pirovano
,
Marcelo E. Domine
,
Patricia Concepción
·
YOU?
·
· 2022
· Open Access
·
· DOI: https://doi.org/10.26434/chemrxiv-2022-l8z6j
YOU?
·
· 2022
· Open Access
·
· DOI: https://doi.org/10.26434/chemrxiv-2022-l8z6j
Enhanced methanol production is obtained over a non-promoted Cu-MgO-Al2O3 mixed oxide catalyst derived from a Cu-Mg-Al hydrotalcite precursor (HT) containing narrowly distributed small Cu NPs (2 nm). Conversions close to the equilibrium (20%) with a methanol selectivity of 67% are achieved at 230 °C, 20 bar and space velocity of 571 mL.gcat-1.h-1. Based on operando spectroscopic studies, the striking activity of this Cu based catalyst is ascribed to the stabilization of Cu+ ions favored under reaction conditions due to lattice reorganization associated with the “HT-memory effect”, promoted by water. Temperature resolved IR-MS experiments have enabled the discernment of monodentate formate species, stabilized on Cu+ as the intermediate in methanol synthesis, in line with the results of DFT calculations. These monodentate formate species are much more reactive than bridge formate species, behaving the last ones as intermediates in methane and CO formation. Moreover, poisoning of the Cu0 surface by strongly adsorbed species behaving as spectators is observed under reaction conditions. This work represents a detailed spectroscopic study highlighting the influence of the reaction pressure on the stabilization of active surface sites, and the possibility of enhancing methanol production on usually less active non-promoted nano-sized copper catalysts, providing that the proper support is selected, allowing the stabilization of doped Cu+. Thus, methanol formation rate of 2.6·10-3molMeOH·gcat-1·h-1 at 230 °C, 20 bar and WHSV = 28500 mL·gcat-1·h-1, is obtained on the Cu-MgO-Al2O3 HT-derived catalyst with 71% methanol selectivity, compared to 2.2·10-4 molMeOH·gcat-1·h-1 with 54% methanol selectivity obtained on a reference Cu/(Al2O3-MgO) catalyst not derived from a HT structure.
Related Topics
Concepts
Methanol
Catalysis
Formate
Chemistry
Copper
Space velocity
Inorganic chemistry
Hydrotalcite
Steam reforming
Selectivity
Adsorption
Physical chemistry
Hydrogen production
Organic chemistry
Metadata
- Type
- preprint
- Language
- en
- Landing Page
- https://doi.org/10.26434/chemrxiv-2022-l8z6j
- https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/621ffe8f91a2e66c5ae2b69d/original/enhanced-methanol-production-over-non-promoted-cu-mg-o-al2o3-materials-with-ex-solved-2-nm-cu-particles-insights-from-an-operando-spectroscopic-study.pdf
- OA Status
- gold
- Cited By
- 3
- References
- 69
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4214924705
All OpenAlex metadata
Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4214924705Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.26434/chemrxiv-2022-l8z6jDigital Object Identifier
- Title
-
Enhanced methanol production over non-promoted Cu-MgO-Al2O3 materials with ex-solved 2 nm Cu particles: Insights from an Operando spectroscopic studyWork title
- Type
-
preprintOpenAlex work type
- Language
-
enPrimary language
- Publication year
-
2022Year of publication
- Publication date
-
2022-03-03Full publication date if available
- Authors
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Jorge Cored, Jaime Mazarío, Cristina Cerdá-Moreno, Pablo G. Lustemberg, M. V. Ganduglia-Pirovano, Marcelo E. Domine, Patricia ConcepciónList of authors in order
- Landing page
-
https://doi.org/10.26434/chemrxiv-2022-l8z6jPublisher landing page
- PDF URL
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https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/621ffe8f91a2e66c5ae2b69d/original/enhanced-methanol-production-over-non-promoted-cu-mg-o-al2o3-materials-with-ex-solved-2-nm-cu-particles-insights-from-an-operando-spectroscopic-study.pdfDirect link to full text PDF
- Open access
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YesWhether a free full text is available
- OA status
-
goldOpen access status per OpenAlex
- OA URL
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https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/621ffe8f91a2e66c5ae2b69d/original/enhanced-methanol-production-over-non-promoted-cu-mg-o-al2o3-materials-with-ex-solved-2-nm-cu-particles-insights-from-an-operando-spectroscopic-study.pdfDirect OA link when available
- Concepts
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Methanol, Catalysis, Formate, Chemistry, Copper, Space velocity, Inorganic chemistry, Hydrotalcite, Steam reforming, Selectivity, Adsorption, Physical chemistry, Hydrogen production, Organic chemistryTop concepts (fields/topics) attached by OpenAlex
- Cited by
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3Total citation count in OpenAlex
- Citations by year (recent)
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2025: 1, 2023: 2Per-year citation counts (last 5 years)
- References (count)
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69Number of works referenced by this work
- Related works (count)
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10Other works algorithmically related by OpenAlex
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