Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell
Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Chen, Chengjie [verfasserIn] Wu, Yinlong [verfasserIn] Li, Xiulan [verfasserIn] Ye, Yanting [verfasserIn] Li, Zilong [verfasserIn] Zhou, Yifan [verfasserIn] Chen, Jian [verfasserIn] Yang, Muzi [verfasserIn] Xie, Fangyan [verfasserIn] Jin, Yanshuo [verfasserIn] Jones, Colton [verfasserIn] Wang, Nan [verfasserIn] Meng, Hui [verfasserIn] Chen, Shaowei [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2023 |
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| Schlagwörter: |
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| Übergeordnetes Werk: |
Enthalten in: Applied catalysis / B - Amsterdam : Elsevier, 1992, 342 |
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| Übergeordnetes Werk: |
volume:342 |
| DOI / URN: |
10.1016/j.apcatb.2023.123407 |
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| Katalog-ID: |
ELV065628349 |
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| 245 | 1 | 0 | |a Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
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| 520 | |a Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. | ||
| 650 | 4 | |a Single atom site | |
| 650 | 4 | |a Few-atom cluster | |
| 650 | 4 | |a Spin state | |
| 650 | 4 | |a Oxygen reduction reaction | |
| 650 | 4 | |a Proton exchange membrane fuel cell | |
| 700 | 1 | |a Wu, Yinlong |e verfasserin |4 aut | |
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| 700 | 1 | |a Meng, Hui |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Shaowei |e verfasserin |0 (orcid)0000-0002-3668-8551 |4 aut | |
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10.1016/j.apcatb.2023.123407 doi (DE-627)ELV065628349 (ELSEVIER)S0926-3373(23)01050-0 DE-627 ger DE-627 rda eng 540 VZ 35.17 bkl 58.50 bkl 43.12 bkl Chen, Chengjie verfasserin aut Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell 2023 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. Single atom site Few-atom cluster Spin state Oxygen reduction reaction Proton exchange membrane fuel cell Wu, Yinlong verfasserin aut Li, Xiulan verfasserin aut Ye, Yanting verfasserin aut Li, Zilong verfasserin aut Zhou, Yifan verfasserin aut Chen, Jian verfasserin aut Yang, Muzi verfasserin aut Xie, Fangyan verfasserin (orcid)0000-0001-5841-7755 aut Jin, Yanshuo verfasserin aut Jones, Colton verfasserin aut Wang, Nan verfasserin aut Meng, Hui verfasserin aut Chen, Shaowei verfasserin (orcid)0000-0002-3668-8551 aut Enthalten in Applied catalysis / B Amsterdam : Elsevier, 1992 342 Online-Ressource (DE-627)320578658 (DE-600)2017331-3 (DE-576)095956344 0926-3373 nnns volume:342 GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 Katalyse VZ 58.50 Umwelttechnik: Allgemeines VZ 43.12 Umweltchemie VZ AR 342 |
| spelling |
10.1016/j.apcatb.2023.123407 doi (DE-627)ELV065628349 (ELSEVIER)S0926-3373(23)01050-0 DE-627 ger DE-627 rda eng 540 VZ 35.17 bkl 58.50 bkl 43.12 bkl Chen, Chengjie verfasserin aut Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell 2023 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. Single atom site Few-atom cluster Spin state Oxygen reduction reaction Proton exchange membrane fuel cell Wu, Yinlong verfasserin aut Li, Xiulan verfasserin aut Ye, Yanting verfasserin aut Li, Zilong verfasserin aut Zhou, Yifan verfasserin aut Chen, Jian verfasserin aut Yang, Muzi verfasserin aut Xie, Fangyan verfasserin (orcid)0000-0001-5841-7755 aut Jin, Yanshuo verfasserin aut Jones, Colton verfasserin aut Wang, Nan verfasserin aut Meng, Hui verfasserin aut Chen, Shaowei verfasserin (orcid)0000-0002-3668-8551 aut Enthalten in Applied catalysis / B Amsterdam : Elsevier, 1992 342 Online-Ressource (DE-627)320578658 (DE-600)2017331-3 (DE-576)095956344 0926-3373 nnns volume:342 GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 Katalyse VZ 58.50 Umwelttechnik: Allgemeines VZ 43.12 Umweltchemie VZ AR 342 |
| allfields_unstemmed |
10.1016/j.apcatb.2023.123407 doi (DE-627)ELV065628349 (ELSEVIER)S0926-3373(23)01050-0 DE-627 ger DE-627 rda eng 540 VZ 35.17 bkl 58.50 bkl 43.12 bkl Chen, Chengjie verfasserin aut Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell 2023 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. Single atom site Few-atom cluster Spin state Oxygen reduction reaction Proton exchange membrane fuel cell Wu, Yinlong verfasserin aut Li, Xiulan verfasserin aut Ye, Yanting verfasserin aut Li, Zilong verfasserin aut Zhou, Yifan verfasserin aut Chen, Jian verfasserin aut Yang, Muzi verfasserin aut Xie, Fangyan verfasserin (orcid)0000-0001-5841-7755 aut Jin, Yanshuo verfasserin aut Jones, Colton verfasserin aut Wang, Nan verfasserin aut Meng, Hui verfasserin aut Chen, Shaowei verfasserin (orcid)0000-0002-3668-8551 aut Enthalten in Applied catalysis / B Amsterdam : Elsevier, 1992 342 Online-Ressource (DE-627)320578658 (DE-600)2017331-3 (DE-576)095956344 0926-3373 nnns volume:342 GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 Katalyse VZ 58.50 Umwelttechnik: Allgemeines VZ 43.12 Umweltchemie VZ AR 342 |
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10.1016/j.apcatb.2023.123407 doi (DE-627)ELV065628349 (ELSEVIER)S0926-3373(23)01050-0 DE-627 ger DE-627 rda eng 540 VZ 35.17 bkl 58.50 bkl 43.12 bkl Chen, Chengjie verfasserin aut Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell 2023 nicht spezifiziert zzz rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. Single atom site Few-atom cluster Spin state Oxygen reduction reaction Proton exchange membrane fuel cell Wu, Yinlong verfasserin aut Li, Xiulan verfasserin aut Ye, Yanting verfasserin aut Li, Zilong verfasserin aut Zhou, Yifan verfasserin aut Chen, Jian verfasserin aut Yang, Muzi verfasserin aut Xie, Fangyan verfasserin (orcid)0000-0001-5841-7755 aut Jin, Yanshuo verfasserin aut Jones, Colton verfasserin aut Wang, Nan verfasserin aut Meng, Hui verfasserin aut Chen, Shaowei verfasserin (orcid)0000-0002-3668-8551 aut Enthalten in Applied catalysis / B Amsterdam : Elsevier, 1992 342 Online-Ressource (DE-627)320578658 (DE-600)2017331-3 (DE-576)095956344 0926-3373 nnns volume:342 GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OLC-PHA GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_150 GBV_ILN_151 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_370 GBV_ILN_602 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2034 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2088 GBV_ILN_2106 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2470 GBV_ILN_2507 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 Katalyse VZ 58.50 Umwelttechnik: Allgemeines VZ 43.12 Umweltchemie VZ AR 342 |
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Chen, Chengjie @@aut@@ Wu, Yinlong @@aut@@ Li, Xiulan @@aut@@ Ye, Yanting @@aut@@ Li, Zilong @@aut@@ Zhou, Yifan @@aut@@ Chen, Jian @@aut@@ Yang, Muzi @@aut@@ Xie, Fangyan @@aut@@ Jin, Yanshuo @@aut@@ Jones, Colton @@aut@@ Wang, Nan @@aut@@ Meng, Hui @@aut@@ Chen, Shaowei @@aut@@ |
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Chen, Chengjie |
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Chen, Chengjie ddc 540 bkl 35.17 bkl 58.50 bkl 43.12 misc Single atom site misc Few-atom cluster misc Spin state misc Oxygen reduction reaction misc Proton exchange membrane fuel cell Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
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540 VZ 35.17 bkl 58.50 bkl 43.12 bkl Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell Single atom site Few-atom cluster Spin state Oxygen reduction reaction Proton exchange membrane fuel cell |
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Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
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Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
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Chen, Chengjie Wu, Yinlong Li, Xiulan Ye, Yanting Li, Zilong Zhou, Yifan Chen, Jian Yang, Muzi Xie, Fangyan Jin, Yanshuo Jones, Colton Wang, Nan Meng, Hui Chen, Shaowei |
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modulating fe spin state in fenc catalysts by adjacent fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
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Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
| abstract |
Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. |
| abstractGer |
Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. |
| abstract_unstemmed |
Iron,nitrogen-codoped carbon (FeNC) has emerged as promising alternatives to precious metals for oxygen reduction reaction (ORR). Herein, we demonstrate that the ORR activity of FeNC can be markedly enhanced by the incorporation of adjacent Fe few-atom clusters (FeAC), where the octahedral field of FeAC boosts the splitting of the parallelogram field of FeN4, and facilitates the transition from high-spin (t2g 3eg 2) Fe(III)N4 to medium-spin (t2g 5eg 1) Fe(II)N4 and hence the interaction with the π* antibonding orbitals of oxygen. This leads to a remarkable ORR performance due to optimized desorption of the OH* intermediate on FeN4, with a half-wave potential of +0.80 in 0.1 M HClO4, in comparison to that with only FeN4 single-atom moieties. In H2-O2 fuel cell tests, a high peak power density of 0.80 W cm−2 is obtained. Results from this work highlight the significance of spin engineering in the manipulation and optimization of the ORR activity of single-atom catalysts. |
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Modulating Fe spin state in FeNC catalysts by adjacent Fe atomic clusters to facilitate oxygen reduction reaction in proton exchange membrane fuel cell |
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Wu, Yinlong Li, Xiulan Ye, Yanting Li, Zilong Zhou, Yifan Chen, Jian Yang, Muzi Xie, Fangyan Jin, Yanshuo Jones, Colton Wang, Nan Meng, Hui Chen, Shaowei |
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