Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode
Operando insights into nickel speciation during nickel-catalyzed cross-electrophile coupling reactions could play a major role in advancing these reactions, but analytical methods capable of providing such insights have not yet been developed. In this study, we integrate a thin-layer electrode (TLE)...
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2025
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| _version_ | 1849927621570199552 |
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| author | Buwanila T. Punchihewa (22688305) |
| author2 | Antonio Romero-Arenas (3110208) Robert S. Paton (1281666) Daniel J. Weix (1284837) Shannon S. Stahl (1291731) Mohammad Rafiee (1474582) |
| author2_role | author author author author author |
| author_facet | Buwanila T. Punchihewa (22688305) Antonio Romero-Arenas (3110208) Robert S. Paton (1281666) Daniel J. Weix (1284837) Shannon S. Stahl (1291731) Mohammad Rafiee (1474582) |
| author_role | author |
| dc.creator.none.fl_str_mv | Buwanila T. Punchihewa (22688305) Antonio Romero-Arenas (3110208) Robert S. Paton (1281666) Daniel J. Weix (1284837) Shannon S. Stahl (1291731) Mohammad Rafiee (1474582) |
| dc.date.none.fl_str_mv | 2025-11-26T09:04:31Z |
| dc.identifier.none.fl_str_mv | 10.1021/jacs.5c12909.s002 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/media/Operando_Analysis_of_Nickel_Catalyst_Speciation_in_Reductive_Biaryl_Synthesis_Using_Thin_Layer_Electrochemistry_and_a_Microelectrode/30719641 |
| dc.rights.none.fl_str_mv | CC BY-NC 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Biochemistry Medicine Ecology Infectious Diseases Environmental Sciences not elsewhere classified Biological Sciences not elsewhere classified analytical methods capable enable operando monitoring ii </ sup nickel catalyst speciation microelectrode operando insights catalyst speciation operando analysis nickel speciation yielding insight temporal evolution results establish reductive homocoupling major role layer electrode kinetic profiles including accumulation different quantities catalyzed cross bipyridyl ligand based intermediates aryl halides approach allows |
| dc.title.none.fl_str_mv | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| dc.type.none.fl_str_mv | Dataset Media info:eu-repo/semantics/publishedVersion dataset |
| description | Operando insights into nickel speciation during nickel-catalyzed cross-electrophile coupling reactions could play a major role in advancing these reactions, but analytical methods capable of providing such insights have not yet been developed. In this study, we integrate a thin-layer electrode (TLE) platform with microelectrode (ME) voltammetry to enable operando monitoring of nickel species during the reductive homocoupling of aryl halides. This approach allows for identification and quantitation of Ni-based intermediates, yielding insight into the temporal evolution of catalyst speciation and their kinetic profiles. The methodology reveals previously unrecognized patterns in nickel speciation, including accumulation of both mono- and bisaryl Ni<sup>II</sup> species during the reactions and variation in the predominant Ni oxidation state (Ni<sup>0</sup>/Ni<sup>II</sup>) with different quantities of the bipyridyl ligand. These results establish the utility of this technique and provide a foundation for its adaptation to other metal-catalyzed reactions. |
| eu_rights_str_mv | openAccess |
| id | Manara_b5fffe877f2ce414d7569f1be3f865e7 |
| identifier_str_mv | 10.1021/jacs.5c12909.s002 |
| network_acronym_str | Manara |
| network_name_str | ManaraRepo |
| oai_identifier_str | oai:figshare.com:article/30719641 |
| publishDate | 2025 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY-NC 4.0 |
| spelling | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a MicroelectrodeBuwanila T. Punchihewa (22688305)Antonio Romero-Arenas (3110208)Robert S. Paton (1281666)Daniel J. Weix (1284837)Shannon S. Stahl (1291731)Mohammad Rafiee (1474582)BiochemistryMedicineEcologyInfectious DiseasesEnvironmental Sciences not elsewhere classifiedBiological Sciences not elsewhere classifiedanalytical methods capableenable operando monitoringii </ supnickel catalyst speciationmicroelectrode operando insightscatalyst speciationoperando analysisnickel speciationyielding insighttemporal evolutionresults establishreductive homocouplingmajor rolelayer electrodekinetic profilesincluding accumulationdifferent quantitiescatalyzed crossbipyridyl ligandbased intermediatesaryl halidesapproach allowsOperando insights into nickel speciation during nickel-catalyzed cross-electrophile coupling reactions could play a major role in advancing these reactions, but analytical methods capable of providing such insights have not yet been developed. In this study, we integrate a thin-layer electrode (TLE) platform with microelectrode (ME) voltammetry to enable operando monitoring of nickel species during the reductive homocoupling of aryl halides. This approach allows for identification and quantitation of Ni-based intermediates, yielding insight into the temporal evolution of catalyst speciation and their kinetic profiles. The methodology reveals previously unrecognized patterns in nickel speciation, including accumulation of both mono- and bisaryl Ni<sup>II</sup> species during the reactions and variation in the predominant Ni oxidation state (Ni<sup>0</sup>/Ni<sup>II</sup>) with different quantities of the bipyridyl ligand. These results establish the utility of this technique and provide a foundation for its adaptation to other metal-catalyzed reactions.2025-11-26T09:04:31ZDatasetMediainfo:eu-repo/semantics/publishedVersiondataset10.1021/jacs.5c12909.s002https://figshare.com/articles/media/Operando_Analysis_of_Nickel_Catalyst_Speciation_in_Reductive_Biaryl_Synthesis_Using_Thin_Layer_Electrochemistry_and_a_Microelectrode/30719641CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/307196412025-11-26T09:04:31Z |
| spellingShingle | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode Buwanila T. Punchihewa (22688305) Biochemistry Medicine Ecology Infectious Diseases Environmental Sciences not elsewhere classified Biological Sciences not elsewhere classified analytical methods capable enable operando monitoring ii </ sup nickel catalyst speciation microelectrode operando insights catalyst speciation operando analysis nickel speciation yielding insight temporal evolution results establish reductive homocoupling major role layer electrode kinetic profiles including accumulation different quantities catalyzed cross bipyridyl ligand based intermediates aryl halides approach allows |
| status_str | publishedVersion |
| title | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| title_full | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| title_fullStr | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| title_full_unstemmed | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| title_short | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| title_sort | Operando Analysis of Nickel Catalyst Speciation in Reductive Biaryl Synthesis Using Thin Layer Electrochemistry and a Microelectrode |
| topic | Biochemistry Medicine Ecology Infectious Diseases Environmental Sciences not elsewhere classified Biological Sciences not elsewhere classified analytical methods capable enable operando monitoring ii </ sup nickel catalyst speciation microelectrode operando insights catalyst speciation operando analysis nickel speciation yielding insight temporal evolution results establish reductive homocoupling major role layer electrode kinetic profiles including accumulation different quantities catalyzed cross bipyridyl ligand based intermediates aryl halides approach allows |