Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites
The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an int...
Ausführliche Beschreibung
Autor*in: |
Li, Xiaoxin [verfasserIn] |
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E-Artikel |
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Englisch |
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2020transfer abstract |
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10 |
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Übergeordnetes Werk: |
Enthalten in: Dynamic patterns of open review process - Zhao, Zhi-Dan ELSEVIER, 2021, an international journal sponsored by the American Carbon Society, Amsterdam [u.a.] |
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Übergeordnetes Werk: |
volume:167 ; year:2020 ; day:15 ; month:10 ; pages:658-667 ; extent:10 |
Links: |
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DOI / URN: |
10.1016/j.carbon.2020.06.036 |
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ELV051161117 |
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520 | |a The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. | ||
520 | |a The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. | ||
650 | 7 | |a Synergistic catalysis |2 Elsevier | |
650 | 7 | |a Graphene |2 Elsevier | |
650 | 7 | |a Single-atom catalyst |2 Elsevier | |
650 | 7 | |a Iron phthalocyanine |2 Elsevier | |
650 | 7 | |a CO2 reduction reaction |2 Elsevier | |
700 | 1 | |a Chai, Guoliang |4 oth | |
700 | 1 | |a Xu, Xiao |4 oth | |
700 | 1 | |a Liu, Jingjing |4 oth | |
700 | 1 | |a Zhong, Zhou |4 oth | |
700 | 1 | |a Cao, Aihui |4 oth | |
700 | 1 | |a Tao, Zhijie |4 oth | |
700 | 1 | |a You, Weifeng |4 oth | |
700 | 1 | |a Kang, Longtian |4 oth | |
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10.1016/j.carbon.2020.06.036 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001112.pica (DE-627)ELV051161117 (ELSEVIER)S0008-6223(20)30603-5 DE-627 ger DE-627 rakwb eng 500 VZ 33.25 bkl 31.00 bkl Li, Xiaoxin verfasserin aut Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites 2020transfer abstract 10 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. Synergistic catalysis Elsevier Graphene Elsevier Single-atom catalyst Elsevier Iron phthalocyanine Elsevier CO2 reduction reaction Elsevier Chai, Guoliang oth Xu, Xiao oth Liu, Jingjing oth Zhong, Zhou oth Cao, Aihui oth Tao, Zhijie oth You, Weifeng oth Kang, Longtian oth Enthalten in Elsevier Science Zhao, Zhi-Dan ELSEVIER Dynamic patterns of open review process 2021 an international journal sponsored by the American Carbon Society Amsterdam [u.a.] (DE-627)ELV006580718 volume:167 year:2020 day:15 month:10 pages:658-667 extent:10 https://doi.org/10.1016/j.carbon.2020.06.036 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OPC-MAT 33.25 Thermodynamik statistische Physik VZ 31.00 Mathematik: Allgemeines VZ AR 167 2020 15 1015 658-667 10 |
spelling |
10.1016/j.carbon.2020.06.036 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001112.pica (DE-627)ELV051161117 (ELSEVIER)S0008-6223(20)30603-5 DE-627 ger DE-627 rakwb eng 500 VZ 33.25 bkl 31.00 bkl Li, Xiaoxin verfasserin aut Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites 2020transfer abstract 10 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. Synergistic catalysis Elsevier Graphene Elsevier Single-atom catalyst Elsevier Iron phthalocyanine Elsevier CO2 reduction reaction Elsevier Chai, Guoliang oth Xu, Xiao oth Liu, Jingjing oth Zhong, Zhou oth Cao, Aihui oth Tao, Zhijie oth You, Weifeng oth Kang, Longtian oth Enthalten in Elsevier Science Zhao, Zhi-Dan ELSEVIER Dynamic patterns of open review process 2021 an international journal sponsored by the American Carbon Society Amsterdam [u.a.] (DE-627)ELV006580718 volume:167 year:2020 day:15 month:10 pages:658-667 extent:10 https://doi.org/10.1016/j.carbon.2020.06.036 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OPC-MAT 33.25 Thermodynamik statistische Physik VZ 31.00 Mathematik: Allgemeines VZ AR 167 2020 15 1015 658-667 10 |
allfields_unstemmed |
10.1016/j.carbon.2020.06.036 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001112.pica (DE-627)ELV051161117 (ELSEVIER)S0008-6223(20)30603-5 DE-627 ger DE-627 rakwb eng 500 VZ 33.25 bkl 31.00 bkl Li, Xiaoxin verfasserin aut Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites 2020transfer abstract 10 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. Synergistic catalysis Elsevier Graphene Elsevier Single-atom catalyst Elsevier Iron phthalocyanine Elsevier CO2 reduction reaction Elsevier Chai, Guoliang oth Xu, Xiao oth Liu, Jingjing oth Zhong, Zhou oth Cao, Aihui oth Tao, Zhijie oth You, Weifeng oth Kang, Longtian oth Enthalten in Elsevier Science Zhao, Zhi-Dan ELSEVIER Dynamic patterns of open review process 2021 an international journal sponsored by the American Carbon Society Amsterdam [u.a.] (DE-627)ELV006580718 volume:167 year:2020 day:15 month:10 pages:658-667 extent:10 https://doi.org/10.1016/j.carbon.2020.06.036 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OPC-MAT 33.25 Thermodynamik statistische Physik VZ 31.00 Mathematik: Allgemeines VZ AR 167 2020 15 1015 658-667 10 |
allfieldsGer |
10.1016/j.carbon.2020.06.036 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001112.pica (DE-627)ELV051161117 (ELSEVIER)S0008-6223(20)30603-5 DE-627 ger DE-627 rakwb eng 500 VZ 33.25 bkl 31.00 bkl Li, Xiaoxin verfasserin aut Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites 2020transfer abstract 10 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. Synergistic catalysis Elsevier Graphene Elsevier Single-atom catalyst Elsevier Iron phthalocyanine Elsevier CO2 reduction reaction Elsevier Chai, Guoliang oth Xu, Xiao oth Liu, Jingjing oth Zhong, Zhou oth Cao, Aihui oth Tao, Zhijie oth You, Weifeng oth Kang, Longtian oth Enthalten in Elsevier Science Zhao, Zhi-Dan ELSEVIER Dynamic patterns of open review process 2021 an international journal sponsored by the American Carbon Society Amsterdam [u.a.] (DE-627)ELV006580718 volume:167 year:2020 day:15 month:10 pages:658-667 extent:10 https://doi.org/10.1016/j.carbon.2020.06.036 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OPC-MAT 33.25 Thermodynamik statistische Physik VZ 31.00 Mathematik: Allgemeines VZ AR 167 2020 15 1015 658-667 10 |
allfieldsSound |
10.1016/j.carbon.2020.06.036 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001112.pica (DE-627)ELV051161117 (ELSEVIER)S0008-6223(20)30603-5 DE-627 ger DE-627 rakwb eng 500 VZ 33.25 bkl 31.00 bkl Li, Xiaoxin verfasserin aut Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites 2020transfer abstract 10 nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. Synergistic catalysis Elsevier Graphene Elsevier Single-atom catalyst Elsevier Iron phthalocyanine Elsevier CO2 reduction reaction Elsevier Chai, Guoliang oth Xu, Xiao oth Liu, Jingjing oth Zhong, Zhou oth Cao, Aihui oth Tao, Zhijie oth You, Weifeng oth Kang, Longtian oth Enthalten in Elsevier Science Zhao, Zhi-Dan ELSEVIER Dynamic patterns of open review process 2021 an international journal sponsored by the American Carbon Society Amsterdam [u.a.] (DE-627)ELV006580718 volume:167 year:2020 day:15 month:10 pages:658-667 extent:10 https://doi.org/10.1016/j.carbon.2020.06.036 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U SSG-OPC-MAT 33.25 Thermodynamik statistische Physik VZ 31.00 Mathematik: Allgemeines VZ AR 167 2020 15 1015 658-667 10 |
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electrocatalytic reduction of co2 to co over iron phthalocyanine-modified graphene nanocomposites |
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Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites |
abstract |
The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. |
abstractGer |
The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. |
abstract_unstemmed |
The non-precious materials with iron-pyrrolic nitrogen-carbon (Fe–N–C) moiety have attracted an increasing attention on the CO2 reduction reaction (CO2RR). However, the influence of iron valence state and environmental synergy is not still clear. Here, iron phthalocyanine (FePc) molecule with an intrinsic Fe–N4–C moiety is enough dispersed on graphene as the single-atom iron catalyst through a facile chemical method. The FePc-graphene composites with different FePc content and iron valence state are synthesized to investigate their catalysis for the CO2RR to CO. The onset overpotential of 190 mV and Faradaic efficiency of >90% may be achieved in the optimal composites. Experimental and calculational results prove the positive role and synergy of Fe(II)Pc with Fe(III)Pc and graphene. The formation of ∗COOH intermediate is confirmed to be the rate-limiting step. The theoretical calculation reveals that Fe(II)Pc should have higher activity than Fe(III)Pc, and Fe(II)Pc/FePc(III) dimer may be better than individual one. This work clearly exhibits the effect of Fe2+/3+- pyrrolic N4–C on the CO2RR. |
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Electrocatalytic reduction of CO2 to CO over iron phthalocyanine-modified graphene nanocomposites |
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