Selective catalysts for the hydrogen oxidation and oxygen reduction reactions by patterning of platinum with calix[4]arene molecules

The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments. The method...

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Published in:	Nature materials Vol. 9; no. 12; pp. 998 - 1003
Main Authors:	Marković, Nenad M, Genorio, Bostjan, Strmcnik, Dusan, Subbaraman, Ram, Tripkovic, Dusan, Karapetrov, Goran, Stamenkovic, Vojislav R, Pejovnik, Stane
Format:	Journal Article
Language:	English
Published:	London Nature Publishing Group UK 01-12-2010 Nature Publishing Group
Subjects:	639/301/299/893 639/301/357 639/301/923/966 Alloy plating Alloying Anodes Biomaterials Carbon Catalysis Catalysts Catalytic oxidation Chemical reactions Chemistry and Materials Science Condensed Matter Physics Electrochemistry Fuel cells Fuel technology Hydrogen letter Materials Science Molecular chemistry Nanotechnology Optical and Electronic Materials Oxidation Oxygen Platinum Polymers Stability
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Abstract	The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments. The methods used to improve catalytic activity are diverse, ranging from the alloying and de-alloying of platinum to the synthesis of platinum core–shell catalysts. However, methods to improve the stability of the carbon supports and catalyst nanoparticles are limited, especially during shutdown (when hydrogen is purged from the anode by air) and startup (when air is purged from the anode by hydrogen) conditions when the cathode potential can be pushed up to 1.5 V (ref. 11). Under the latter conditions, stability of the cathode materials is strongly affected (carbon oxidation reaction) by the undesired oxygen reduction reaction (ORR) on the anode side. This emphasizes the importance of designing selective anode catalysts that can efficiently suppress the ORR while fully preserving the Pt-like activity for the hydrogen oxidation reaction. Here, we demonstrate that chemically modified platinum with a self-assembled monolayer of calix[4]arene molecules meets this challenging requirement.
AbstractList	Cathode degradation and methods for improving the selectivity of anode catalysts remain crucial challenges for the design of polymer electrolyte membrane fuel cells. A chemically modified Pt electrode with a self-assembled monolayer of calix[4]arene molecules is now shown to selectively block the undesired oxygen reduction reaction. The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments 1 , 2 . The methods used to improve catalytic activity are diverse 3 , 4 , 5 , 6 , 7 , 8 , ranging from the alloying 3 , 4 and de-alloying 5 of platinum to the synthesis of platinum core–shell catalysts 6 . However, methods to improve the stability of the carbon supports and catalyst nanoparticles are limited 9 , 10 , especially during shutdown (when hydrogen is purged from the anode by air) and startup (when air is purged from the anode by hydrogen) conditions when the cathode potential can be pushed up to 1.5 V (ref. 11 ). Under the latter conditions, stability of the cathode materials is strongly affected (carbon oxidation reaction) by the undesired oxygen reduction reaction (ORR) on the anode side. This emphasizes the importance of designing selective anode catalysts that can efficiently suppress the ORR while fully preserving the Pt-like activity for the hydrogen oxidation reaction. Here, we demonstrate that chemically modified platinum with a self-assembled monolayer of calix[4]arene molecules meets this challenging requirement. The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments. The methods used to improve catalytic activity are diverse, ranging from the alloying and de-alloying of platinum to the synthesis of platinum core–shell catalysts. However, methods to improve the stability of the carbon supports and catalyst nanoparticles are limited, especially during shutdown (when hydrogen is purged from the anode by air) and startup (when air is purged from the anode by hydrogen) conditions when the cathode potential can be pushed up to 1.5 V (ref. 11). Under the latter conditions, stability of the cathode materials is strongly affected (carbon oxidation reaction) by the undesired oxygen reduction reaction (ORR) on the anode side. This emphasizes the importance of designing selective anode catalysts that can efficiently suppress the ORR while fully preserving the Pt-like activity for the hydrogen oxidation reaction. Here, we demonstrate that chemically modified platinum with a self-assembled monolayer of calix[4]arene molecules meets this challenging requirement. The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments. The methods used to improve catalytic activity are diverse, ranging from the alloying and de-alloying of platinum to the synthesis of platinum core-shell catalysts. However, methods to improve the stability of the carbon supports and catalyst nanoparticles are limited, especially during shutdown (when hydrogen is purged from the anode by air) and startup (when air is purged from the anode by hydrogen) conditions when the cathode potential can be pushed up to 1.5 V (ref. 11). Under the latter conditions, stability of the cathode materials is strongly affected (carbon oxidation reaction) by the undesired oxygen reduction reaction (ORR) on the anode side. This emphasizes the importance of designing selective anode catalysts that can efficiently suppress the ORR while fully preserving the Pt-like activity for the hydrogen oxidation reaction. Here, we demonstrate that chemically modified platinum with a self-assembled monolayer of calix[4]arene molecules meets this challenging requirement. The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments. The methods used to improve catalytic activity are diverse, ranging from the alloying and de-alloying of platinum to the synthesis of platinum core-shell catalysts. However, methods to improve the stability of the carbon supports and catalyst nanoparticles are limited, especially during shutdown (when hydrogen is purged from the anode by air) and startup (when air is purged from the anode by hydrogen) conditions when the cathode potential can be pushed up to 1.5V (ref.11). Under the latter conditions, stability of the cathode materials is strongly affected (carbon oxidation reaction) by the undesired oxygen reduction reaction (ORR) on the anode side. This emphasizes the importance of designing selective anode catalysts that can efficiently suppress the ORR while fully preserving the Pt-like activity for the hydrogen oxidation reaction. Here, we demonstrate that chemically modified platinum with a self-assembled monolayer of calix[4]arene molecules meets this challenging requirement. The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their catalytic behaviour as well as the long-term stability of the metal catalysts and supports in hostile electrochemical environments1, 2. The methods used to improve catalytic activity are diverse3, 4, 5, 6, 7, 8, ranging from the alloying3, 4 and de-alloying5 of platinum to the synthesis of platinum core-shell catalysts6. However, methods to improve the stability of the carbon supports and catalyst nanoparticles are limited9, 10, especially during shutdown (when hydrogen is purged from the anode by air) and startup (when air is purged from the anode by hydrogen) conditions when the cathode potential can be pushed up to 1.5 V (ref. 11). Under the latter conditions, stability of the cathode materials is strongly affected (carbon oxidation reaction) by the undesired oxygen reduction reaction (ORR) on the anode side. This emphasizes the importance of designing selective anode catalysts that can efficiently suppress the ORR while fully preserving the Pt-like activity for the hydrogen oxidation reaction. Here, we demonstrate that chemically modified platinum with a self-assembled monolayer of calix[4]arene molecules meets this challenging requirement. [PUBLICATION ABSTRACT]
Author	Strmcnik, Dusan Karapetrov, Goran Stamenkovic, Vojislav R Genorio, Bostjan Pejovnik, Stane Marković, Nenad M Subbaraman, Ram Tripkovic, Dusan
Author_xml	– sequence: 1 givenname: Nenad M surname: Marković fullname: Marković, Nenad M organization: Materials Science Division, Argonne National Laboratory – sequence: 2 givenname: Bostjan surname: Genorio fullname: Genorio, Bostjan organization: Faculty of Chemistry and Chemical Technology, University of Ljubljana National Institute of Chemistry – sequence: 3 givenname: Dusan surname: Strmcnik fullname: Strmcnik, Dusan organization: Materials Science Division, Argonne National Laboratory – sequence: 4 givenname: Ram surname: Subbaraman fullname: Subbaraman, Ram organization: Nuclear Engineering Division, Argonne National Laboratory – sequence: 5 givenname: Dusan surname: Tripkovic fullname: Tripkovic, Dusan organization: Materials Science Division, Argonne National Laboratory – sequence: 6 givenname: Goran surname: Karapetrov fullname: Karapetrov, Goran organization: Materials Science Division, Argonne National Laboratory – sequence: 7 givenname: Vojislav R surname: Stamenkovic fullname: Stamenkovic, Vojislav R organization: Materials Science Division, Argonne National Laboratory – sequence: 8 givenname: Stane surname: Pejovnik fullname: Pejovnik, Stane organization: Faculty of Chemistry and Chemical Technology, University of Ljubljana
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Snippet	The design of new catalysts for polymer electrolyte membrane fuel cells must be guided by two equally important fundamental principles: optimization of their... Cathode degradation and methods for improving the selectivity of anode catalysts remain crucial challenges for the design of polymer electrolyte membrane fuel...
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SubjectTerms	639/301/299/893 639/301/357 639/301/923/966 Alloy plating Alloying Anodes Biomaterials Carbon Catalysis Catalysts Catalytic oxidation Chemical reactions Chemistry and Materials Science Condensed Matter Physics Electrochemistry Fuel cells Fuel technology Hydrogen letter Materials Science Molecular chemistry Nanotechnology Optical and Electronic Materials Oxidation Oxygen Platinum Polymers Stability
Title	Selective catalysts for the hydrogen oxidation and oxygen reduction reactions by patterning of platinum with calix[4]arene molecules
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