Tuning the Spin State of the Iron Center by Bridge-Bonded Fe-O-Ti Ligands for Enhanced Oxygen Reduction

Yarong Liu; Xiangjian Liu; Zunhang Lv; Rui Liu; Liuhua Li; Jinming Wang; Wenxiu Yang; Xin Jiang; Xiao Feng; Bo Wang

doi:10.1002/anie.202117617

Tuning the Spin State of the Iron Center by Bridge-Bonded Fe-O-Ti Ligands for Enhanced Oxygen Reduction

Yarong Liu, Xiangjian Liu, Zunhang Lv, Rui Liu, Liuhua Li, Jinming Wang, Wenxiu Yang^*, Xin Jiang^*, Xiao Feng, Bo Wang^*

^*Corresponding author for this work

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

116 Citations (Scopus)

Abstract

Exploring functional substrates and precisely regulating the electronic structures of atomic metal active species with moderate spin state are of great importance yet remain challenging. Hereon, we provide an axial Fe-O-Ti ligand regulated spin-state transition strategy to improve the oxygen reduction reaction (ORR) activity of Fe centers. Theoretical calculations indicate that Fe-O-Ti ligands in FeN₃O-O-Ti can induce a low-to-medium spin-state transition and optimize O₂ adsorption by FeN₃O. As a proof-of-concept, the oriented catalyst was prepared from atomic-Fe-doped polymer-like quantum dots and ultrathin o-terminated MXene. The optimal catalyst exhibits an intrinsic activity that is almost 5 times higher than the control sample (without axial Fe-O-Ti ligands). It also delivers a superior performance in Zn-air batteries and H₂/O₂ anion exchange membrane fuel cells in a wide-temperature range.

Original language	English
Article number	e202117617
Journal	Angewandte Chemie - International Edition
Volume	61
Issue number	21
DOIs	https://doi.org/10.1002/anie.202117617
Publication status	Published - 16 May 2022

Keywords

Axial Coordination
Electrocatalysis
Oxygen Reduction Reaction
Single-Atom Catalyst
Spin-State Tuning

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10.1002/anie.202117617

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title = "Tuning the Spin State of the Iron Center by Bridge-Bonded Fe-O-Ti Ligands for Enhanced Oxygen Reduction",

abstract = "Exploring functional substrates and precisely regulating the electronic structures of atomic metal active species with moderate spin state are of great importance yet remain challenging. Hereon, we provide an axial Fe-O-Ti ligand regulated spin-state transition strategy to improve the oxygen reduction reaction (ORR) activity of Fe centers. Theoretical calculations indicate that Fe-O-Ti ligands in FeN3O-O-Ti can induce a low-to-medium spin-state transition and optimize O2 adsorption by FeN3O. As a proof-of-concept, the oriented catalyst was prepared from atomic-Fe-doped polymer-like quantum dots and ultrathin o-terminated MXene. The optimal catalyst exhibits an intrinsic activity that is almost 5 times higher than the control sample (without axial Fe-O-Ti ligands). It also delivers a superior performance in Zn-air batteries and H2/O2 anion exchange membrane fuel cells in a wide-temperature range.",

keywords = "Axial Coordination, Electrocatalysis, Oxygen Reduction Reaction, Single-Atom Catalyst, Spin-State Tuning",

author = "Yarong Liu and Xiangjian Liu and Zunhang Lv and Rui Liu and Liuhua Li and Jinming Wang and Wenxiu Yang and Xin Jiang and Xiao Feng and Bo Wang",

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year = "2022",

month = may,

day = "16",

doi = "10.1002/anie.202117617",

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T1 - Tuning the Spin State of the Iron Center by Bridge-Bonded Fe-O-Ti Ligands for Enhanced Oxygen Reduction

AU - Liu, Yarong

AU - Liu, Xiangjian

AU - Lv, Zunhang

AU - Liu, Rui

AU - Li, Liuhua

AU - Wang, Jinming

AU - Yang, Wenxiu

AU - Jiang, Xin

AU - Feng, Xiao

AU - Wang, Bo

PY - 2022/5/16

Y1 - 2022/5/16

N2 - Exploring functional substrates and precisely regulating the electronic structures of atomic metal active species with moderate spin state are of great importance yet remain challenging. Hereon, we provide an axial Fe-O-Ti ligand regulated spin-state transition strategy to improve the oxygen reduction reaction (ORR) activity of Fe centers. Theoretical calculations indicate that Fe-O-Ti ligands in FeN3O-O-Ti can induce a low-to-medium spin-state transition and optimize O2 adsorption by FeN3O. As a proof-of-concept, the oriented catalyst was prepared from atomic-Fe-doped polymer-like quantum dots and ultrathin o-terminated MXene. The optimal catalyst exhibits an intrinsic activity that is almost 5 times higher than the control sample (without axial Fe-O-Ti ligands). It also delivers a superior performance in Zn-air batteries and H2/O2 anion exchange membrane fuel cells in a wide-temperature range.

AB - Exploring functional substrates and precisely regulating the electronic structures of atomic metal active species with moderate spin state are of great importance yet remain challenging. Hereon, we provide an axial Fe-O-Ti ligand regulated spin-state transition strategy to improve the oxygen reduction reaction (ORR) activity of Fe centers. Theoretical calculations indicate that Fe-O-Ti ligands in FeN3O-O-Ti can induce a low-to-medium spin-state transition and optimize O2 adsorption by FeN3O. As a proof-of-concept, the oriented catalyst was prepared from atomic-Fe-doped polymer-like quantum dots and ultrathin o-terminated MXene. The optimal catalyst exhibits an intrinsic activity that is almost 5 times higher than the control sample (without axial Fe-O-Ti ligands). It also delivers a superior performance in Zn-air batteries and H2/O2 anion exchange membrane fuel cells in a wide-temperature range.

KW - Axial Coordination

KW - Electrocatalysis

KW - Oxygen Reduction Reaction

KW - Single-Atom Catalyst

KW - Spin-State Tuning

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SN - 1433-7851

VL - 61

JO - Angewandte Chemie - International Edition

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M1 - e202117617

ER -

Tuning the Spin State of the Iron Center by Bridge-Bonded Fe-O-Ti Ligands for Enhanced Oxygen Reduction

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Keywords

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