Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst

<p dir="ltr">Dimethyl carbonate (DMC) has emerged as a promising candidate for sustainable chemical processes due to its remarkable versatility and low toxicity. From a green chemistry perspective, the direct synthesis of DMC has been considered the most promising route, as water is...

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التفاصيل البيبلوغرافية
المؤلف الرئيسي: G. Ibrahim (7601063) (author)
مؤلفون آخرون: A. Abdelbar (22155280) (author), H. A. Choudhury (4427449) (author), M. S. Challiwala (22155283) (author), A. Prakash (2247199) (author), K. Mondal (2610661) (author), S. Solim (22155286) (author), Nimir O. Elbashir (1850563) (author)
منشور في: 2024
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author G. Ibrahim (7601063)
author2 A. Abdelbar (22155280)
H. A. Choudhury (4427449)
M. S. Challiwala (22155283)
A. Prakash (2247199)
K. Mondal (2610661)
S. Solim (22155286)
Nimir O. Elbashir (1850563)
author2_role author
author
author
author
author
author
author
author_facet G. Ibrahim (7601063)
A. Abdelbar (22155280)
H. A. Choudhury (4427449)
M. S. Challiwala (22155283)
A. Prakash (2247199)
K. Mondal (2610661)
S. Solim (22155286)
Nimir O. Elbashir (1850563)
author_role author
dc.creator.none.fl_str_mv G. Ibrahim (7601063)
A. Abdelbar (22155280)
H. A. Choudhury (4427449)
M. S. Challiwala (22155283)
A. Prakash (2247199)
K. Mondal (2610661)
S. Solim (22155286)
Nimir O. Elbashir (1850563)
dc.date.none.fl_str_mv 2024-09-03T03:00:00Z
dc.identifier.none.fl_str_mv 10.1007/s11244-024-02003-w
dc.relation.none.fl_str_mv https://figshare.com/articles/journal_contribution/Experimental_Verification_of_Low-Pressure_Kinetics_Model_for_Direct_Synthesis_of_Dimethyl_Carbonate_Over_CeO_sub_2_sub_Catalyst/30023407
dc.rights.none.fl_str_mv CC BY 4.0
info:eu-repo/semantics/openAccess
dc.subject.none.fl_str_mv Engineering
Chemical engineering
Environmental sciences
Environmental management
CO2 conversion
Kinetics model
CeO2-catalysts
Direct DMC synthesis
CO2Fix
Sustainable processes
Mean absolute percentage error
dc.title.none.fl_str_mv Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
dc.type.none.fl_str_mv Text
Journal contribution
info:eu-repo/semantics/publishedVersion
text
contribution to journal
description <p dir="ltr">Dimethyl carbonate (DMC) has emerged as a promising candidate for sustainable chemical processes due to its remarkable versatility and low toxicity. From a green chemistry perspective, the direct synthesis of DMC has been considered the most promising route, as water is the only byproduct generated in the reaction between CO<sub>2</sub> and methanol. However, this synthetic route has faced significant thermodynamic limitations, even at elevated pressure conditions. Therefore, a two-part study explored low-pressure synthesis of DMC via the direct route, and a low-pressure kinetic model for the CeO<sub>2</sub> catalyst was developed based on the results. Proposed Langmuir–Hinshelwood mechanisms were verified using experimental data generated in our labs. The investigation suggests that DMC formation in the direct synthetic route is a surface reaction of CO<sub>2</sub> and methanol on the catalyst. The kinetic model predictions closely aligned with experimental data, demonstrating a 17% mean absolute percentage error and indicating a high level of predictability. Additionally, a rigorous assessment was conducted on CO<sub>2</sub> fixations in DMC synthesis, quantifying CO<sub>2</sub> capture and its conversion into stable or high-value products, formally designated as CO<sub>2</sub> Fixation (CO2Fix). The CO<sub>2</sub>Fix analysis revealed that, at a conversion rate of 27%, the process can achieve a "net zero" state when operated at an approximate pressure of 30 bar, thereby supporting the viability of low-pressure synthesis. Increasing the conversion rate to levels exceeding 95% significantly enhances the CO<sub>2</sub>Fix metric, potentially surpassing 3.5 or higher.</p><h2>Other Information</h2><p dir="ltr">Published in: Topics in Catalysis<br>License: <a href="https://creativecommons.org/licenses/by/4.0" target="_blank">https://creativecommons.org/licenses/by/4.0</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1007/s11244-024-02003-w" target="_blank">https://dx.doi.org/10.1007/s11244-024-02003-w</a></p>
eu_rights_str_mv openAccess
id Manara2_3b459ce41684128d406aa054e303d4ff
identifier_str_mv 10.1007/s11244-024-02003-w
network_acronym_str Manara2
network_name_str Manara2
oai_identifier_str oai:figshare.com:article/30023407
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spelling Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> CatalystG. Ibrahim (7601063)A. Abdelbar (22155280)H. A. Choudhury (4427449)M. S. Challiwala (22155283)A. Prakash (2247199)K. Mondal (2610661)S. Solim (22155286)Nimir O. Elbashir (1850563)EngineeringChemical engineeringEnvironmental sciencesEnvironmental managementCO2 conversionKinetics modelCeO2-catalystsDirect DMC synthesisCO2FixSustainable processesMean absolute percentage error<p dir="ltr">Dimethyl carbonate (DMC) has emerged as a promising candidate for sustainable chemical processes due to its remarkable versatility and low toxicity. From a green chemistry perspective, the direct synthesis of DMC has been considered the most promising route, as water is the only byproduct generated in the reaction between CO<sub>2</sub> and methanol. However, this synthetic route has faced significant thermodynamic limitations, even at elevated pressure conditions. Therefore, a two-part study explored low-pressure synthesis of DMC via the direct route, and a low-pressure kinetic model for the CeO<sub>2</sub> catalyst was developed based on the results. Proposed Langmuir–Hinshelwood mechanisms were verified using experimental data generated in our labs. The investigation suggests that DMC formation in the direct synthetic route is a surface reaction of CO<sub>2</sub> and methanol on the catalyst. The kinetic model predictions closely aligned with experimental data, demonstrating a 17% mean absolute percentage error and indicating a high level of predictability. Additionally, a rigorous assessment was conducted on CO<sub>2</sub> fixations in DMC synthesis, quantifying CO<sub>2</sub> capture and its conversion into stable or high-value products, formally designated as CO<sub>2</sub> Fixation (CO2Fix). The CO<sub>2</sub>Fix analysis revealed that, at a conversion rate of 27%, the process can achieve a "net zero" state when operated at an approximate pressure of 30 bar, thereby supporting the viability of low-pressure synthesis. Increasing the conversion rate to levels exceeding 95% significantly enhances the CO<sub>2</sub>Fix metric, potentially surpassing 3.5 or higher.</p><h2>Other Information</h2><p dir="ltr">Published in: Topics in Catalysis<br>License: <a href="https://creativecommons.org/licenses/by/4.0" target="_blank">https://creativecommons.org/licenses/by/4.0</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1007/s11244-024-02003-w" target="_blank">https://dx.doi.org/10.1007/s11244-024-02003-w</a></p>2024-09-03T03:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.1007/s11244-024-02003-whttps://figshare.com/articles/journal_contribution/Experimental_Verification_of_Low-Pressure_Kinetics_Model_for_Direct_Synthesis_of_Dimethyl_Carbonate_Over_CeO_sub_2_sub_Catalyst/30023407CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/300234072024-09-03T03:00:00Z
spellingShingle Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
G. Ibrahim (7601063)
Engineering
Chemical engineering
Environmental sciences
Environmental management
CO2 conversion
Kinetics model
CeO2-catalysts
Direct DMC synthesis
CO2Fix
Sustainable processes
Mean absolute percentage error
status_str publishedVersion
title Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
title_full Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
title_fullStr Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
title_full_unstemmed Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
title_short Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
title_sort Experimental Verification of Low-Pressure Kinetics Model for Direct Synthesis of Dimethyl Carbonate Over CeO<sub>2</sub> Catalyst
topic Engineering
Chemical engineering
Environmental sciences
Environmental management
CO2 conversion
Kinetics model
CeO2-catalysts
Direct DMC synthesis
CO2Fix
Sustainable processes
Mean absolute percentage error