Engineering Fe–Fe3C@Fe–N–C Active Sites and Hybrid Structures from Dual Metal–Organic Frameworks for Oxygen Reduction Reaction in H2–O2 Fuel Cell and Li–O2 Battery

Dual metal–organic frameworks (MOFs, i.e., MIL‐100(Fe) and ZIF‐8) are thermally converted into Fe–Fe3C‐embedded Fe–N‐codoped carbon as platinum group metal (PGM)‐free oxygen reduction reaction (ORR) electrocatalysts. Pyrolysis enables imidazolate in ZIF‐8 rearranged into highly N‐doped carbon, while...

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Vydané v:	Advanced functional materials Ročník 29; číslo 23
Hlavní autori:	Wang, Hao, Yin, Feng‐Xiang, Liu, Ning, Kou, Rong‐Hui, He, Xiao‐Bo, Sun, Cheng‐Jun, Chen, Biao‐Hua, Liu, Di‐Jia, Yin, Hua‐Qiang
Médium:	Journal Article
Jazyk:	English
Vydavateľské údaje:	Hoboken Wiley Subscription Services, Inc 06.06.2019
Predmet:	Amorphous materials Batteries Carbon Catalysis Catalysts Cementite Charge transfer Computer simulation Electrocatalysts Fuel cells Graphitization H2–O2 fuel cell Hybrid structures Iron carbides iron–nitrogen–carbon Li–O2 battery Materials science Metal-organic frameworks Nanoparticles oxygen reduction reaction Oxygen reduction reactions Platinum Proton exchange membrane fuel cells Pyrolysis
ISSN:	1616-301X, 1616-3028
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Abstract	Dual metal–organic frameworks (MOFs, i.e., MIL‐100(Fe) and ZIF‐8) are thermally converted into Fe–Fe3C‐embedded Fe–N‐codoped carbon as platinum group metal (PGM)‐free oxygen reduction reaction (ORR) electrocatalysts. Pyrolysis enables imidazolate in ZIF‐8 rearranged into highly N‐doped carbon, while Fe from MIL‐100(Fe) into N‐ligated atomic sites concurrently with a few Fe–Fe3C nanoparticles. Upon precise control of MOF compositions, the optimal catalyst is highly active for the ORR in half‐cells (0.88 V in base and 0.79 V versus RHE in acid in half‐wave potential), a proton exchange membrane fuel cell (0.76 W cm−2 in peak power density) and an aprotic Li–O2 battery (8749 mAh g−1 in discharge capacity), representing a state‐of‐the‐art PGM‐free ORR catalyst. In the material, amorphous carbon with partial graphitization ensures high active site exposure and fast charge transfer simultaneously. Macropores facilitate mass transport to the catalyst surface, followed by oxygen penetration in micropores to reach the infiltrated active sites. Further modeling simulations shed light on the true Fe–Fe3C contribution to the catalyst performance, suggesting Fe3C enhances oxygen affinity, while metallic Fe promotes *OH desorption as the rate‐determining step at the nearby Fe–N–C sites. These findings demonstrate MOFs as model system for rational design of electrocatalyst for energy‐based functional applications. An Fe–N–C catalyst is derived from dual metal–organic frameworks through facile pyrolysis, affording excellent oxygen reduction catalytic performance in alkaline/acidic half‐cells, a H2–O2 proton exchange membrane fuel cell, and a Li–O2 battery. The excellent catalytic performance benefits from density populated Fe–Fe3C@Fe–N–C dual active sites, hierarchical porosities for mass transport, and partial carbon graphitization for charge transfer.
AbstractList	Dual metal–organic frameworks (MOFs, i.e., MIL‐100(Fe) and ZIF‐8) are thermally converted into Fe–Fe3C‐embedded Fe–N‐codoped carbon as platinum group metal (PGM)‐free oxygen reduction reaction (ORR) electrocatalysts. Pyrolysis enables imidazolate in ZIF‐8 rearranged into highly N‐doped carbon, while Fe from MIL‐100(Fe) into N‐ligated atomic sites concurrently with a few Fe–Fe3C nanoparticles. Upon precise control of MOF compositions, the optimal catalyst is highly active for the ORR in half‐cells (0.88 V in base and 0.79 V versus RHE in acid in half‐wave potential), a proton exchange membrane fuel cell (0.76 W cm−2 in peak power density) and an aprotic Li–O2 battery (8749 mAh g−1 in discharge capacity), representing a state‐of‐the‐art PGM‐free ORR catalyst. In the material, amorphous carbon with partial graphitization ensures high active site exposure and fast charge transfer simultaneously. Macropores facilitate mass transport to the catalyst surface, followed by oxygen penetration in micropores to reach the infiltrated active sites. Further modeling simulations shed light on the true Fe–Fe3C contribution to the catalyst performance, suggesting Fe3C enhances oxygen affinity, while metallic Fe promotes OH desorption as the rate‐determining step at the nearby Fe–N–C sites. These findings demonstrate MOFs as model system for rational design of electrocatalyst for energy‐based functional applications. Dual metal–organic frameworks (MOFs, i.e., MIL‐100(Fe) and ZIF‐8) are thermally converted into Fe–Fe3C‐embedded Fe–N‐codoped carbon as platinum group metal (PGM)‐free oxygen reduction reaction (ORR) electrocatalysts. Pyrolysis enables imidazolate in ZIF‐8 rearranged into highly N‐doped carbon, while Fe from MIL‐100(Fe) into N‐ligated atomic sites concurrently with a few Fe–Fe3C nanoparticles. Upon precise control of MOF compositions, the optimal catalyst is highly active for the ORR in half‐cells (0.88 V in base and 0.79 V versus RHE in acid in half‐wave potential), a proton exchange membrane fuel cell (0.76 W cm−2 in peak power density) and an aprotic Li–O2 battery (8749 mAh g−1 in discharge capacity), representing a state‐of‐the‐art PGM‐free ORR catalyst. In the material, amorphous carbon with partial graphitization ensures high active site exposure and fast charge transfer simultaneously. Macropores facilitate mass transport to the catalyst surface, followed by oxygen penetration in micropores to reach the infiltrated active sites. Further modeling simulations shed light on the true Fe–Fe3C contribution to the catalyst performance, suggesting Fe3C enhances oxygen affinity, while metallic Fe promotes OH desorption as the rate‐determining step at the nearby Fe–N–C sites. These findings demonstrate MOFs as model system for rational design of electrocatalyst for energy‐based functional applications. An Fe–N–C catalyst is derived from dual metal–organic frameworks through facile pyrolysis, affording excellent oxygen reduction catalytic performance in alkaline/acidic half‐cells, a H2–O2 proton exchange membrane fuel cell, and a Li–O2 battery. The excellent catalytic performance benefits from density populated Fe–Fe3C@Fe–N–C dual active sites, hierarchical porosities for mass transport, and partial carbon graphitization for charge transfer.
Author	Liu, Ning Kou, Rong‐Hui Yin, Hua‐Qiang Sun, Cheng‐Jun Liu, Di‐Jia He, Xiao‐Bo Chen, Biao‐Hua Yin, Feng‐Xiang Wang, Hao
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SubjectTerms	Amorphous materials Batteries Carbon Catalysis Catalysts Cementite Charge transfer Computer simulation Electrocatalysts Fuel cells Graphitization H2–O2 fuel cell Hybrid structures Iron carbides iron–nitrogen–carbon Li–O2 battery Materials science Metal-organic frameworks Nanoparticles oxygen reduction reaction Oxygen reduction reactions Platinum Proton exchange membrane fuel cells Pyrolysis
Title	Engineering Fe–Fe3C@Fe–N–C Active Sites and Hybrid Structures from Dual Metal–Organic Frameworks for Oxygen Reduction Reaction in H2–O2 Fuel Cell and Li–O2 Battery
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