DC Field | Value | Language |
---|---|---|
dc.contributor.author | Choi, Chang Hyuck | ko |
dc.contributor.author | Lim, Hyung Kyu | ko |
dc.contributor.author | Chung, Min Wook | ko |
dc.contributor.author | Chon, Gajeon | ko |
dc.contributor.author | Sahraie, Nastaran Ranjbar | ko |
dc.contributor.author | Altin, Abdulrahman | ko |
dc.contributor.author | Sougrati, Moulay-Tahar | ko |
dc.contributor.author | Stievano, Lorenzo | ko |
dc.contributor.author | Oh, Hyun Seok | ko |
dc.contributor.author | Park, Eun Soo | ko |
dc.contributor.author | Luo, Fang | ko |
dc.contributor.author | Strasser, Peter | ko |
dc.contributor.author | Drazic, Goran | ko |
dc.contributor.author | Mayrhofer, Karl J. J. | ko |
dc.contributor.author | Kim, Hyungjun | ko |
dc.contributor.author | Jaouen, Frederic | ko |
dc.date.accessioned | 2018-12-20T05:10:10Z | - |
dc.date.available | 2018-12-20T05:10:10Z | - |
dc.date.created | 2018-12-03 | - |
dc.date.created | 2018-12-03 | - |
dc.date.issued | 2018-11 | - |
dc.identifier.citation | ENERGY & ENVIRONMENTAL SCIENCE, v.11, no.11, pp.3176 - 3182 | - |
dc.identifier.issn | 1754-5692 | - |
dc.identifier.uri | http://hdl.handle.net/10203/247620 | - |
dc.description.abstract | For catalysing dioxygen reduction, iron-nitrogen-carbon (Fe-N-C) materials are today the best candidates to replace platinum in proton-exchange membrane fuel cell (PEMFC) cathodes. Despite tremendous progress in their activity and site-structure understanding, improved durability is critically needed but challenged by insufficient understanding of their degradation mechanisms during operation. Here, we show that FeNxCy moieties in a representative Fe-N-C catalyst are structurally stable but electrochemically unstable when exposed in an acidic medium to H2O2, the main oxygen reduction reaction (ORR) byproduct. We reveal that exposure to H2O2 leaves iron-based catalytic sites untouched but decreases their turnover frequency (TOF) via oxidation of the carbon surface, leading to weakened O-2-binding on iron-based sites. Their TOF is recovered upon electrochemical reduction of the carbon surface, demonstrating the proposed deactivation mechanism. Our results reveal for the first time a hitherto unsuspected key deactivation mechanism during the ORR in an acidic medium. This study identifies the N-doped carbon surface as the Achilles' heel during ORR catalysis in PEMFCs. Observed in acidic but not in alkaline electrolytes, these insights suggest that durable Fe-N-C catalysts are within reach for PEMFCs if rational strategies minimizing the amount of H2O2 or reactive oxygen species (ROS) produced during the ORR are developed. | - |
dc.language | English | - |
dc.publisher | ROYAL SOC CHEMISTRY | - |
dc.title | The Achilles' heel of iron-based catalysts during oxygen reduction in an acidic medium | - |
dc.type | Article | - |
dc.identifier.wosid | 000449843300008 | - |
dc.identifier.scopusid | 2-s2.0-85056769239 | - |
dc.type.rims | ART | - |
dc.citation.volume | 11 | - |
dc.citation.issue | 11 | - |
dc.citation.beginningpage | 3176 | - |
dc.citation.endingpage | 3182 | - |
dc.citation.publicationname | ENERGY & ENVIRONMENTAL SCIENCE | - |
dc.identifier.doi | 10.1039/c8ee01855c | - |
dc.contributor.localauthor | Kim, Hyungjun | - |
dc.contributor.nonIdAuthor | Choi, Chang Hyuck | - |
dc.contributor.nonIdAuthor | Chung, Min Wook | - |
dc.contributor.nonIdAuthor | Chon, Gajeon | - |
dc.contributor.nonIdAuthor | Sahraie, Nastaran Ranjbar | - |
dc.contributor.nonIdAuthor | Altin, Abdulrahman | - |
dc.contributor.nonIdAuthor | Sougrati, Moulay-Tahar | - |
dc.contributor.nonIdAuthor | Stievano, Lorenzo | - |
dc.contributor.nonIdAuthor | Oh, Hyun Seok | - |
dc.contributor.nonIdAuthor | Park, Eun Soo | - |
dc.contributor.nonIdAuthor | Luo, Fang | - |
dc.contributor.nonIdAuthor | Strasser, Peter | - |
dc.contributor.nonIdAuthor | Drazic, Goran | - |
dc.contributor.nonIdAuthor | Mayrhofer, Karl J. J. | - |
dc.contributor.nonIdAuthor | Jaouen, Frederic | - |
dc.description.isOpenAccess | N | - |
dc.type.journalArticle | Article | - |
dc.subject.keywordPlus | NITROGEN-DOPED CARBON | - |
dc.subject.keywordPlus | MEMBRANE FUEL-CELLS | - |
dc.subject.keywordPlus | FE/N/C CATALYSTS | - |
dc.subject.keywordPlus | WORK FUNCTION | - |
dc.subject.keywordPlus | ACTIVE-SITES | - |
dc.subject.keywordPlus | GRAPHENE | - |
dc.subject.keywordPlus | ELECTROCATALYSTS | - |
dc.subject.keywordPlus | IDENTIFICATION | - |
dc.subject.keywordPlus | STABILITY | - |
dc.subject.keywordPlus | ORR | - |
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