Enhanced photocatalytic hydrogen evolution with a Mixed-Valence iron Metal-Organic framework

Xinning Zhang; Xiaojie Ma; Yuqing Ye; Caixia Guo; Xiaojun Xu; Junwen Zhou; Bo Wang

doi:10.1016/j.cej.2022.140939

Enhanced photocatalytic hydrogen evolution with a Mixed-Valence iron Metal-Organic framework

Xinning Zhang, Xiaojie Ma^*, Yuqing Ye, Caixia Guo, Xiaojun Xu, Junwen Zhou, Bo Wang

^*Corresponding author for this work

School of Chemistry and Chemical Engineering

Beijing Institute of Technology

Research output: Contribution to journal › Article › peer-review

10 Citations (Scopus)

Abstract

Fe-oxo cluster-based metal–organic frameworks (MOFs) offer a tunable platform for visible-light-driven catalysis, yet the unmatched energy level and the ease of charge recombination strongly hinder their application in photocatalytic H₂ generation. In this work, we report an Fe(II/III) mixed-valence catalyst derived from the transition of an Fe(II)₂N₂O₁₀ cluster-based MOF in water through a solvent displacement pathway. Both electronic band structure and charge transfer dynamics are effectively optimized via heteroatom coordination and valence mixing in the iron clusters. 25 times the visible-light-induced H₂ yield of pristine FeMOF was obtained by Fe(II/III) MOF with platinum as cocatalyst. The Fe MOF catalyst also shows significantly superior performance in comparison with the well-known oxide catalyst α-Fe₂O₃ and the commonly investigated MOF catalyst NH₂-UiO-66. This work provides a direction for the structural engineering of Fe-MOFs for photocatalysts.

Original language	English
Article number	140939
Journal	Chemical Engineering Journal
Volume	456
DOIs	https://doi.org/10.1016/j.cej.2022.140939
Publication status	Published - 15 Jan 2023

Keywords

Heteroatom coordination
Hydrogen evolution
Iron metal–organic framework
Mixed-valence
Photocatalyst

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10.1016/j.cej.2022.140939

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title = "Enhanced photocatalytic hydrogen evolution with a Mixed-Valence iron Metal-Organic framework",

abstract = "Fe-oxo cluster-based metal–organic frameworks (MOFs) offer a tunable platform for visible-light-driven catalysis, yet the unmatched energy level and the ease of charge recombination strongly hinder their application in photocatalytic H2 generation. In this work, we report an Fe(II/III) mixed-valence catalyst derived from the transition of an Fe(II)2N2O10 cluster-based MOF in water through a solvent displacement pathway. Both electronic band structure and charge transfer dynamics are effectively optimized via heteroatom coordination and valence mixing in the iron clusters. 25 times the visible-light-induced H2 yield of pristine FeMOF was obtained by Fe(II/III) MOF with platinum as cocatalyst. The Fe MOF catalyst also shows significantly superior performance in comparison with the well-known oxide catalyst α-Fe2O3 and the commonly investigated MOF catalyst NH2-UiO-66. This work provides a direction for the structural engineering of Fe-MOFs for photocatalysts.",

keywords = "Heteroatom coordination, Hydrogen evolution, Iron metal–organic framework, Mixed-valence, Photocatalyst",

author = "Xinning Zhang and Xiaojie Ma and Yuqing Ye and Caixia Guo and Xiaojun Xu and Junwen Zhou and Bo Wang",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2023",

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doi = "10.1016/j.cej.2022.140939",

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T1 - Enhanced photocatalytic hydrogen evolution with a Mixed-Valence iron Metal-Organic framework

AU - Zhang, Xinning

AU - Ma, Xiaojie

AU - Ye, Yuqing

AU - Guo, Caixia

AU - Xu, Xiaojun

AU - Zhou, Junwen

AU - Wang, Bo

PY - 2023/1/15

Y1 - 2023/1/15

N2 - Fe-oxo cluster-based metal–organic frameworks (MOFs) offer a tunable platform for visible-light-driven catalysis, yet the unmatched energy level and the ease of charge recombination strongly hinder their application in photocatalytic H2 generation. In this work, we report an Fe(II/III) mixed-valence catalyst derived from the transition of an Fe(II)2N2O10 cluster-based MOF in water through a solvent displacement pathway. Both electronic band structure and charge transfer dynamics are effectively optimized via heteroatom coordination and valence mixing in the iron clusters. 25 times the visible-light-induced H2 yield of pristine FeMOF was obtained by Fe(II/III) MOF with platinum as cocatalyst. The Fe MOF catalyst also shows significantly superior performance in comparison with the well-known oxide catalyst α-Fe2O3 and the commonly investigated MOF catalyst NH2-UiO-66. This work provides a direction for the structural engineering of Fe-MOFs for photocatalysts.

AB - Fe-oxo cluster-based metal–organic frameworks (MOFs) offer a tunable platform for visible-light-driven catalysis, yet the unmatched energy level and the ease of charge recombination strongly hinder their application in photocatalytic H2 generation. In this work, we report an Fe(II/III) mixed-valence catalyst derived from the transition of an Fe(II)2N2O10 cluster-based MOF in water through a solvent displacement pathway. Both electronic band structure and charge transfer dynamics are effectively optimized via heteroatom coordination and valence mixing in the iron clusters. 25 times the visible-light-induced H2 yield of pristine FeMOF was obtained by Fe(II/III) MOF with platinum as cocatalyst. The Fe MOF catalyst also shows significantly superior performance in comparison with the well-known oxide catalyst α-Fe2O3 and the commonly investigated MOF catalyst NH2-UiO-66. This work provides a direction for the structural engineering of Fe-MOFs for photocatalysts.

KW - Heteroatom coordination

KW - Hydrogen evolution

KW - Iron metal–organic framework

KW - Mixed-valence

KW - Photocatalyst

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DO - 10.1016/j.cej.2022.140939

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SN - 1385-8947

VL - 456

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

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ER -

Enhanced photocatalytic hydrogen evolution with a Mixed-Valence iron Metal-Organic framework

Abstract

Keywords

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