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

^*此作品的通讯作者

化学与化工学院

Beijing Institute of Technology

科研成果: 期刊稿件 › 文章 › 同行评审

10 引用（Scopus）

摘要

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.

源语言	英语
文章编号	140939
期刊	Chemical Engineering Journal
卷	456
DOI	https://doi.org/10.1016/j.cej.2022.140939
出版状态	已出版 - 15 1月 2023

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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",

month = jan,

day = "15",

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

language = "English",

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TY - JOUR

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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U2 - 10.1016/j.cej.2022.140939

DO - 10.1016/j.cej.2022.140939

M3 - Article

AN - SCOPUS:85144555678

SN - 1385-8947

VL - 456

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

M1 - 140939

ER -

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

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