Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance
<p dir="ltr">Density functional theory (DFT) calculations have been utilized to evaluate the complete reaction mechanism of methane dry reforming (DRM) over Ni2Cu (111) bimetallic catalyst. The detailed catalytic cycle on Ni<sub>2</sub>Cu (111) catalyst demonstrated super...
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2020
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| _version_ | 1864513511805157376 |
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| author | Ahmed Omran (9269789) |
| author2 | Sun Hee Yoon (7179263) Murtaza Khan (6550739) Minhaj Ghouri (18806869) Anjaneyulu Chatla (4888933) Nimir Elbashir (5244551) |
| author2_role | author author author author author |
| author_facet | Ahmed Omran (9269789) Sun Hee Yoon (7179263) Murtaza Khan (6550739) Minhaj Ghouri (18806869) Anjaneyulu Chatla (4888933) Nimir Elbashir (5244551) |
| author_role | author |
| dc.creator.none.fl_str_mv | Ahmed Omran (9269789) Sun Hee Yoon (7179263) Murtaza Khan (6550739) Minhaj Ghouri (18806869) Anjaneyulu Chatla (4888933) Nimir Elbashir (5244551) |
| dc.date.none.fl_str_mv | 2020-09-10T06:00:00Z |
| dc.identifier.none.fl_str_mv | 10.3390/catal10091043 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/journal_contribution/Mechanistic_Insights_for_Dry_Reforming_of_Methane_on_Cu_Ni_Bimetallic_Catalysts_DFT-Assisted_Microkinetic_Analysis_for_Coke_Resistance/26114545 |
| dc.rights.none.fl_str_mv | CC BY 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Chemical sciences Physical chemistry Engineering Chemical engineering density functional theory (DFT) dry reforming of methane (DRM) Ni2Cu (111) bimetallic catalyst coke resistance catalyst deactivation and microkinetic |
| dc.title.none.fl_str_mv | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| dc.type.none.fl_str_mv | Text Journal contribution info:eu-repo/semantics/publishedVersion text contribution to journal |
| description | <p dir="ltr">Density functional theory (DFT) calculations have been utilized to evaluate the complete reaction mechanism of methane dry reforming (DRM) over Ni2Cu (111) bimetallic catalyst. The detailed catalytic cycle on Ni<sub>2</sub>Cu (111) catalyst demonstrated superior coke resistance compared to pure Ni (111) and Ni2Fe (111) reported in the literature. Doping Cu in the Ni–Ni network enhanced the competitive CH oxidation by both atomic O and OH species with the latter having only 0.02 eV higher than the 1.06 eV energy barrier required for CH oxidation by atomic O. Among the C/CH oxidation pathways, C* + O* → CO (g) was the most favorable with an energy barrier of 0.72 eV. This was almost half of the energy barrier required for the rate-limiting step of CH decomposition (1.40 eV) and indicated enhanced coke deposition removal. Finally, we investigated the effect of temperature (800~1000 K) on the carbon deposition and elimination mechanism over Ni<sub>2</sub>Cu (111) catalyst. Under those realistic DRM conditions, the calculations showed a periodic cycle of simultaneous carbon deposition and elimination resulting in improved catalyst stability.</p><h2>Other Information</h2><p dir="ltr">Published in: Catalysts<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/10.3390/catal10091043" target="_blank">https://dx.doi.org/10.3390/catal10091043</a></p><p dir="ltr">Additional institutions affiliated with: Chemical Engineering Program - TAMUQ</p> |
| eu_rights_str_mv | openAccess |
| id | Manara2_92a11e4ff3de4d3d25e1a8abb6d74d94 |
| identifier_str_mv | 10.3390/catal10091043 |
| network_acronym_str | Manara2 |
| network_name_str | Manara2 |
| oai_identifier_str | oai:figshare.com:article/26114545 |
| publishDate | 2020 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY 4.0 |
| spelling | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke ResistanceAhmed Omran (9269789)Sun Hee Yoon (7179263)Murtaza Khan (6550739)Minhaj Ghouri (18806869)Anjaneyulu Chatla (4888933)Nimir Elbashir (5244551)Chemical sciencesPhysical chemistryEngineeringChemical engineeringdensity functional theory (DFT)dry reforming of methane (DRM)Ni2Cu (111)bimetallic catalystcoke resistancecatalyst deactivationand microkinetic<p dir="ltr">Density functional theory (DFT) calculations have been utilized to evaluate the complete reaction mechanism of methane dry reforming (DRM) over Ni2Cu (111) bimetallic catalyst. The detailed catalytic cycle on Ni<sub>2</sub>Cu (111) catalyst demonstrated superior coke resistance compared to pure Ni (111) and Ni2Fe (111) reported in the literature. Doping Cu in the Ni–Ni network enhanced the competitive CH oxidation by both atomic O and OH species with the latter having only 0.02 eV higher than the 1.06 eV energy barrier required for CH oxidation by atomic O. Among the C/CH oxidation pathways, C* + O* → CO (g) was the most favorable with an energy barrier of 0.72 eV. This was almost half of the energy barrier required for the rate-limiting step of CH decomposition (1.40 eV) and indicated enhanced coke deposition removal. Finally, we investigated the effect of temperature (800~1000 K) on the carbon deposition and elimination mechanism over Ni<sub>2</sub>Cu (111) catalyst. Under those realistic DRM conditions, the calculations showed a periodic cycle of simultaneous carbon deposition and elimination resulting in improved catalyst stability.</p><h2>Other Information</h2><p dir="ltr">Published in: Catalysts<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/10.3390/catal10091043" target="_blank">https://dx.doi.org/10.3390/catal10091043</a></p><p dir="ltr">Additional institutions affiliated with: Chemical Engineering Program - TAMUQ</p>2020-09-10T06:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.3390/catal10091043https://figshare.com/articles/journal_contribution/Mechanistic_Insights_for_Dry_Reforming_of_Methane_on_Cu_Ni_Bimetallic_Catalysts_DFT-Assisted_Microkinetic_Analysis_for_Coke_Resistance/26114545CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/261145452020-09-10T06:00:00Z |
| spellingShingle | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance Ahmed Omran (9269789) Chemical sciences Physical chemistry Engineering Chemical engineering density functional theory (DFT) dry reforming of methane (DRM) Ni2Cu (111) bimetallic catalyst coke resistance catalyst deactivation and microkinetic |
| status_str | publishedVersion |
| title | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| title_full | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| title_fullStr | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| title_full_unstemmed | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| title_short | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| title_sort | Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance |
| topic | Chemical sciences Physical chemistry Engineering Chemical engineering density functional theory (DFT) dry reforming of methane (DRM) Ni2Cu (111) bimetallic catalyst coke resistance catalyst deactivation and microkinetic |