Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids
The oxygen reduction reaction (ORR) in aqueous media plays a critical role in sustainable and clean energy technologies such as polymer electrolyte membrane and alkaline fuel cells. In this work, we present a new concept to improve the ORR performance by engineering the interface reaction at the electrocatalyst/electrolyte/oxygen triple-phase boundary using a protic and hydrophobic ionic liquid and demonstrate the wide and general applicability of this concept to several Pt-free catalysts. Two catalysts, Fe–N codoped and metal-free N-doped carbon electrocatalysts, are used as a proof of concept. The ionic liquid layer grafted at the nanocarbon surface creates a water-equilibrated secondary reaction medium with a higher O2 affinity toward oxygen adsorption, promoting the diffusion toward the catalytic active site, while its protic character provides sufficient H+/H3O+ conductivity, and the hydrophobic nature prevents the resulting reaction product water from accumulating and blocking the interface. Our strategy brings obvious improvements in the ORR performance in both acid and alkaline electrolytes, while the catalytic activity of FeNC-nanocarbon outperforms commercial Pt–C in alkaline electrolytes. We believe that this research will pave new routes toward the development of high-performance ORR catalysts free of noble metals via careful interface engineering at the triple point.
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American Chemical Society
2019
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Subjects: | non-precious metal catalysts, electrocatalysis, triple phase boundary, interface reaction, oxygen reduction reaction, |
Online Access: | http://hdl.handle.net/10261/223514 |
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dig-incar-es-10261-2235142020-12-10T15:44:28Z Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids Qiao, Mo Álvarez Ferrero, Guillermo Fernández Velasco, Leticia Vern Hor, Wei Yang, Yan Luo, Hui Lodewyckx, Peter Fuertes Arias, Antonio Benito Sevilla Solís, Marta Titirici, María-Magdalena non-precious metal catalysts electrocatalysis triple phase boundary interface reaction oxygen reduction reaction The oxygen reduction reaction (ORR) in aqueous media plays a critical role in sustainable and clean energy technologies such as polymer electrolyte membrane and alkaline fuel cells. In this work, we present a new concept to improve the ORR performance by engineering the interface reaction at the electrocatalyst/electrolyte/oxygen triple-phase boundary using a protic and hydrophobic ionic liquid and demonstrate the wide and general applicability of this concept to several Pt-free catalysts. Two catalysts, Fe–N codoped and metal-free N-doped carbon electrocatalysts, are used as a proof of concept. The ionic liquid layer grafted at the nanocarbon surface creates a water-equilibrated secondary reaction medium with a higher O2 affinity toward oxygen adsorption, promoting the diffusion toward the catalytic active site, while its protic character provides sufficient H+/H3O+ conductivity, and the hydrophobic nature prevents the resulting reaction product water from accumulating and blocking the interface. Our strategy brings obvious improvements in the ORR performance in both acid and alkaline electrolytes, while the catalytic activity of FeNC-nanocarbon outperforms commercial Pt–C in alkaline electrolytes. We believe that this research will pave new routes toward the development of high-performance ORR catalysts free of noble metals via careful interface engineering at the triple point. M.-M.T. would like to acknowledge EPSRC grants EP/R021554/1 and EP/N509899/1 and the EU CIG 631092. M.Q., Y.Y., H.L. acknowledge the CSC for a PhD scholarship. Professor Maria-Magdalena Titirici was founded by: EPSRC EP/S018204/1, EPSRC EP/R021554/1, and EPSRC EP/N509899/1. 2020-11-23T14:50:04Z 2020-11-23T14:50:04Z 2019 2020-11-23T14:50:04Z artículo http://purl.org/coar/resource_type/c_6501 doi: 10.1021/acsami.8b18375 issn: 1944-8252 ACS Applied Materials and Interfaces 11: 11298- 11305 (2019) http://hdl.handle.net/10261/223514 10.1021/acsami.8b18375 http://dx.doi.org/10.1021/acsami.8b18375 Sí none American Chemical Society |
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non-precious metal catalysts electrocatalysis triple phase boundary interface reaction oxygen reduction reaction non-precious metal catalysts electrocatalysis triple phase boundary interface reaction oxygen reduction reaction |
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non-precious metal catalysts electrocatalysis triple phase boundary interface reaction oxygen reduction reaction non-precious metal catalysts electrocatalysis triple phase boundary interface reaction oxygen reduction reaction Qiao, Mo Álvarez Ferrero, Guillermo Fernández Velasco, Leticia Vern Hor, Wei Yang, Yan Luo, Hui Lodewyckx, Peter Fuertes Arias, Antonio Benito Sevilla Solís, Marta Titirici, María-Magdalena Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids |
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The oxygen reduction reaction (ORR) in aqueous media plays a critical role in sustainable and clean energy technologies such as polymer electrolyte membrane and alkaline fuel cells. In this work, we present a new concept to improve the ORR performance by engineering the interface reaction at the electrocatalyst/electrolyte/oxygen triple-phase boundary using a protic and hydrophobic ionic liquid and demonstrate the wide and general applicability of this concept to several Pt-free catalysts. Two catalysts, Fe–N codoped and metal-free N-doped carbon electrocatalysts, are used as a proof of concept. The ionic liquid layer grafted at the nanocarbon surface creates a water-equilibrated secondary reaction medium with a higher O2 affinity toward oxygen adsorption, promoting the diffusion toward the catalytic active site, while its protic character provides sufficient H+/H3O+ conductivity, and the hydrophobic nature prevents the resulting reaction product water from accumulating and blocking the interface. Our strategy brings obvious improvements in the ORR performance in both acid and alkaline electrolytes, while the catalytic activity of FeNC-nanocarbon outperforms commercial Pt–C in alkaline electrolytes. We believe that this research will pave new routes toward the development of high-performance ORR catalysts free of noble metals via careful interface engineering at the triple point. |
format |
artículo |
topic_facet |
non-precious metal catalysts electrocatalysis triple phase boundary interface reaction oxygen reduction reaction |
author |
Qiao, Mo Álvarez Ferrero, Guillermo Fernández Velasco, Leticia Vern Hor, Wei Yang, Yan Luo, Hui Lodewyckx, Peter Fuertes Arias, Antonio Benito Sevilla Solís, Marta Titirici, María-Magdalena |
author_facet |
Qiao, Mo Álvarez Ferrero, Guillermo Fernández Velasco, Leticia Vern Hor, Wei Yang, Yan Luo, Hui Lodewyckx, Peter Fuertes Arias, Antonio Benito Sevilla Solís, Marta Titirici, María-Magdalena |
author_sort |
Qiao, Mo |
title |
Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids |
title_short |
Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids |
title_full |
Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids |
title_fullStr |
Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids |
title_full_unstemmed |
Boosting the Oxygen Reduction Electrocatalytic Performance of Nonprecious Metal Nanocarbons via Triple Boundary Engineering Using Protic Ionic Liquids |
title_sort |
boosting the oxygen reduction electrocatalytic performance of nonprecious metal nanocarbons via triple boundary engineering using protic ionic liquids |
publisher |
American Chemical Society |
publishDate |
2019 |
url |
http://hdl.handle.net/10261/223514 |
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