Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts
At the initial stage of the oxygen evolution reaction (OER) most electrocatalysts undergo structural and chemical surface reconstruction. While this reconstruction strongly influences their performance, it is frequently overlooked. Herein, we analyze the role of the oxidized anions, which is particu...
| Autores: | ; ; ; ; ; ; ; ; ; ; |
|---|---|
| Tipo de documento: | Artículo |
| Fecha de publicación: | 2023 |
| País: | España |
| Institución: | Universitat Politècnica de Catalunya (UPC) |
| Repositorio: | UPCommons. Portal del coneixement obert de la UPC |
| Lenguaje: | Inglés |
| OAI Identifier: | oai:upcommons.upc.edu:2117/387857 |
| Acceso en línea: | https://hdl.handle.net/2117/387857 https://dx.doi.org/10.1016/j.apcatb.2022.121988 |
| Nivel de acceso: | Acceso abierto |
| Palabra clave: | Catalysis Amorphous oxide Anion adsorption Structural reconstruction Leaching Oxygen evolution reaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| _version_ | 1878738982303432704 |
|---|---|
| author | Wang, Xiang |
| author2 | Xu, Han Du, Ruifeng Liang, Zhifu Zuo, Yong Guardia, Pablo Li, Junshan Llorca Piqué, Jordi|||0000-0002-7447-9582 Arbiol Cobos, Jordi Zheng, Renji Cabot, Andreu |
| author2_role | author author author author author author author author author author |
| author_browse | Arbiol Cobos, Jordi Cabot, Andreu Du, Ruifeng Guardia, Pablo Li, Junshan Liang, Zhifu Llorca Piqué, Jordi|||0000-0002-7447-9582 Wang, Xiang Xu, Han Zheng, Renji Zuo, Yong |
| author_facet | Wang, Xiang Xu, Han Du, Ruifeng Liang, Zhifu Zuo, Yong Guardia, Pablo Li, Junshan Llorca Piqué, Jordi|||0000-0002-7447-9582 Arbiol Cobos, Jordi Zheng, Renji Cabot, Andreu |
| author_role | author |
| collection | UPCommons. Portal del coneixement obert de la UPC |
| description | At the initial stage of the oxygen evolution reaction (OER) most electrocatalysts undergo structural and chemical surface reconstruction. While this reconstruction strongly influences their performance, it is frequently overlooked. Herein, we analyze the role of the oxidized anions, which is particularly neglected in most previous works. We introduce a range of different anionic groups (Cl-, CH3COO-, NO3-, SO42-) on the surface of an amorphous ZnCoxNiyOz catalyst by a facile proton etching and ion exchange method from a ZIF-8 self-sacrificial template. The structural and chemical properties of the obtained set of materials are thoroughly analysed and correlated with their electrocatalytic performance to study the effect of surface anionic groups, phase transition, metal leaching and defect generation on OER activity. Exploiting the control possibilities provided by the synthesis method here described and employing the uncovered property-performance correlations, the electrocatalyst is optimized. As a result, we produce ZnCo1.25Ni0.73Ox-SO4 catalysts with outstanding OER performances, including a low overpotential of 252 mV at 10 mA cm-2 with a small Tafel slope of 41.6 mV dec-1. Furthermore, this catalyst exhibits remarkable stability with negligible overpotential variation for 100 h. The excellent catalytic properties are rationalized using density functional theory calculations, showing that the surface-adsorbed anions, particularly SO42-, can stabilize the OOH* intermediate, thus enhancing the OER activity. This work o¿ers new insight into the roles of metal leaching and surface-adsorbed anions in the OER progress and facilitates the rational design of highly-efficient electrocatalysts for OER. |
| eu_rights_str_mv | openAccess |
| format | article |
| id | ES_b8d117defa46a1e2cf32eba3cfcfaa96 |
| institution | Universitat Politècnica de Catalunya (UPC) |
| instname_str | Universitat Politècnica de Catalunya (UPC) |
| language | eng |
| network_acronym_str | ES |
| network_name_str | España |
| oai_identifier_str | oai:upcommons.upc.edu:2117/387857 |
| publishDate | 2023 |
| publishDateSort | 2023 |
| publisher | Elsevier |
| publisherStr | Elsevier |
| reponame_str | UPCommons. Portal del coneixement obert de la UPC |
| spelling | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts Wang, Xiang Xu, Han Du, Ruifeng Liang, Zhifu Zuo, Yong Guardia, Pablo Li, Junshan Llorca Piqué, Jordi|||0000-0002-7447-9582 Arbiol Cobos, Jordi Zheng, Renji Cabot, Andreu Catalysis Amorphous oxide Anion adsorption Structural reconstruction Leaching Oxygen evolution reaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química At the initial stage of the oxygen evolution reaction (OER) most electrocatalysts undergo structural and chemical surface reconstruction. While this reconstruction strongly influences their performance, it is frequently overlooked. Herein, we analyze the role of the oxidized anions, which is particularly neglected in most previous works. We introduce a range of different anionic groups (Cl-, CH3COO-, NO3-, SO42-) on the surface of an amorphous ZnCoxNiyOz catalyst by a facile proton etching and ion exchange method from a ZIF-8 self-sacrificial template. The structural and chemical properties of the obtained set of materials are thoroughly analysed and correlated with their electrocatalytic performance to study the effect of surface anionic groups, phase transition, metal leaching and defect generation on OER activity. Exploiting the control possibilities provided by the synthesis method here described and employing the uncovered property-performance correlations, the electrocatalyst is optimized. As a result, we produce ZnCo1.25Ni0.73Ox-SO4 catalysts with outstanding OER performances, including a low overpotential of 252 mV at 10 mA cm-2 with a small Tafel slope of 41.6 mV dec-1. Furthermore, this catalyst exhibits remarkable stability with negligible overpotential variation for 100 h. The excellent catalytic properties are rationalized using density functional theory calculations, showing that the surface-adsorbed anions, particularly SO42-, can stabilize the OOH* intermediate, thus enhancing the OER activity. This work o¿ers new insight into the roles of metal leaching and surface-adsorbed anions in the OER progress and facilitates the rational design of highly-efficient electrocatalysts for OER. Peer Reviewed Elsevier https://hdl.handle.net/2117/387857 https://dx.doi.org/10.1016/j.apcatb.2022.121988 |
| spellingShingle | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts Wang, Xiang Catalysis Amorphous oxide Anion adsorption Structural reconstruction Leaching Oxygen evolution reaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| title | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts |
| title_full | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts |
| title_fullStr | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts |
| title_full_unstemmed | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts |
| title_short | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts |
| title_sort | Unveiling the role of counter-anions in amorphous transition metal-based oxygen evolution electrocatalysts |
| topic | Catalysis Amorphous oxide Anion adsorption Structural reconstruction Leaching Oxygen evolution reaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| topic_facet | Catalysis Amorphous oxide Anion adsorption Structural reconstruction Leaching Oxygen evolution reaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| url | https://hdl.handle.net/2117/387857 https://dx.doi.org/10.1016/j.apcatb.2022.121988 |