An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane
<p dir="ltr">The influence of varying Cu atomic ratios in a bimetallic Ni-Cu catalytic system for the CO<sub>2</sub> or Dry Reforming of Methane (DRM) is investigated experimentally, in conjunction with <i>ab-initio</i> Density Functional Theory (DFT) and Gene...
Saved in:
| Main Author: | |
|---|---|
| Other Authors: | , , , , |
| Published: |
2020
|
| Subjects: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1864513558766682112 |
|---|---|
| author | Anjaneyulu Chatla (4888933) |
| author2 | Minhaj M. Ghouri (17115637) Omar Wissam El Hassan (17115640) Nosaiba Mohamed (17115643) Anuj V. Prakash (17115646) Nimir O. Elbashir (1850563) |
| author2_role | author author author author author |
| author_facet | Anjaneyulu Chatla (4888933) Minhaj M. Ghouri (17115637) Omar Wissam El Hassan (17115640) Nosaiba Mohamed (17115643) Anuj V. Prakash (17115646) Nimir O. Elbashir (1850563) |
| author_role | author |
| dc.creator.none.fl_str_mv | Anjaneyulu Chatla (4888933) Minhaj M. Ghouri (17115637) Omar Wissam El Hassan (17115640) Nosaiba Mohamed (17115643) Anuj V. Prakash (17115646) Nimir O. Elbashir (1850563) |
| dc.date.none.fl_str_mv | 2020-07-25T00:00:00Z |
| dc.identifier.none.fl_str_mv | 10.1016/j.apcata.2020.117699 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/journal_contribution/An_experimental_and_first_principles_DFT_investigation_on_the_effect_of_Cu_addition_to_Ni_Al_sub_2_sub_O_sub_3_sub_catalyst_for_the_dry_reforming_of_methane/24270343 |
| dc.rights.none.fl_str_mv | CC BY 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Engineering Chemical engineering Resources engineering and extractive metallurgy DRM Ni-Cu alloy DFT Generalized Power Law Expression (GPLE) Bi-metallic catalyst Catalyst deactivation |
| dc.title.none.fl_str_mv | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| dc.type.none.fl_str_mv | Text Journal contribution info:eu-repo/semantics/publishedVersion text contribution to journal |
| description | <p dir="ltr">The influence of varying Cu atomic ratios in a bimetallic Ni-Cu catalytic system for the CO<sub>2</sub> or Dry Reforming of Methane (DRM) is investigated experimentally, in conjunction with <i>ab-initio</i> Density Functional Theory (DFT) and Generalized Power Law Expression (GPLE)-based mathematical modeling approaches. Among the synthesized catalysts, an 8:1 Ni:Cu ratio shows highest activity with stable H<sub>2</sub>/CO selectivity compared to its monometallic counterpart. Detailed physico-chemical characterization of the catalysts indicate that copper addition minimizes deactivation by forming a Ni-Cu alloy that increases reducibility of the NiO and limits the tendency of the active site toward coke formation. DFT calculations reveal increased energy barrier for carbon adsorption, whilst promoting facile removal of deposited carbon. GPLE analysis of the deactivation profiles suggest coking as the primary deactivation route in monometallic Ni catalyst; although much lesser in extent, deactivation of Ni<sub>8</sub>Cu<sub>1</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst is induced by both sintering and coking regimes.</p><h2>Other Information</h2><p dir="ltr">Published in: Applied Catalysis A: General<br>License: <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">http://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1016/j.apcata.2020.117699" target="_blank">https://dx.doi.org/10.1016/j.apcata.2020.117699</a></p> |
| eu_rights_str_mv | openAccess |
| id | Manara2_1b22574fc6922f0fa8451d9404c9e573 |
| identifier_str_mv | 10.1016/j.apcata.2020.117699 |
| network_acronym_str | Manara2 |
| network_name_str | Manara2 |
| oai_identifier_str | oai:figshare.com:article/24270343 |
| publishDate | 2020 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY 4.0 |
| spelling | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methaneAnjaneyulu Chatla (4888933)Minhaj M. Ghouri (17115637)Omar Wissam El Hassan (17115640)Nosaiba Mohamed (17115643)Anuj V. Prakash (17115646)Nimir O. Elbashir (1850563)EngineeringChemical engineeringResources engineering and extractive metallurgyDRMNi-Cu alloyDFTGeneralized Power Law Expression (GPLE)Bi-metallic catalystCatalyst deactivation<p dir="ltr">The influence of varying Cu atomic ratios in a bimetallic Ni-Cu catalytic system for the CO<sub>2</sub> or Dry Reforming of Methane (DRM) is investigated experimentally, in conjunction with <i>ab-initio</i> Density Functional Theory (DFT) and Generalized Power Law Expression (GPLE)-based mathematical modeling approaches. Among the synthesized catalysts, an 8:1 Ni:Cu ratio shows highest activity with stable H<sub>2</sub>/CO selectivity compared to its monometallic counterpart. Detailed physico-chemical characterization of the catalysts indicate that copper addition minimizes deactivation by forming a Ni-Cu alloy that increases reducibility of the NiO and limits the tendency of the active site toward coke formation. DFT calculations reveal increased energy barrier for carbon adsorption, whilst promoting facile removal of deposited carbon. GPLE analysis of the deactivation profiles suggest coking as the primary deactivation route in monometallic Ni catalyst; although much lesser in extent, deactivation of Ni<sub>8</sub>Cu<sub>1</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst is induced by both sintering and coking regimes.</p><h2>Other Information</h2><p dir="ltr">Published in: Applied Catalysis A: General<br>License: <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">http://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1016/j.apcata.2020.117699" target="_blank">https://dx.doi.org/10.1016/j.apcata.2020.117699</a></p>2020-07-25T00:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.1016/j.apcata.2020.117699https://figshare.com/articles/journal_contribution/An_experimental_and_first_principles_DFT_investigation_on_the_effect_of_Cu_addition_to_Ni_Al_sub_2_sub_O_sub_3_sub_catalyst_for_the_dry_reforming_of_methane/24270343CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/242703432020-07-25T00:00:00Z |
| spellingShingle | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane Anjaneyulu Chatla (4888933) Engineering Chemical engineering Resources engineering and extractive metallurgy DRM Ni-Cu alloy DFT Generalized Power Law Expression (GPLE) Bi-metallic catalyst Catalyst deactivation |
| status_str | publishedVersion |
| title | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| title_full | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| title_fullStr | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| title_full_unstemmed | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| title_short | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| title_sort | An experimental and first principles DFT investigation on the effect of Cu addition to Ni/Al<sub>2</sub>O<sub>3</sub> catalyst for the dry reforming of methane |
| topic | Engineering Chemical engineering Resources engineering and extractive metallurgy DRM Ni-Cu alloy DFT Generalized Power Law Expression (GPLE) Bi-metallic catalyst Catalyst deactivation |