Depletable peroxidase-like activity of Fe3O4 nanozymes accompanied with separate migration of electrons and iron ions

As pioneering Fe 3 O 4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe 2+ -induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution...

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Veröffentlicht in:	Nature communications Jg. 13; H. 1; S. 5365 - 11
Hauptverfasser:	Dong, Haijiao, Du, Wei, Dong, Jian, Che, Renchao, Kong, Fei, Cheng, Wenlong, Ma, Ming, Gu, Ning, Zhang, Yu
Format:	Journal Article
Sprache:	Englisch
Veröffentlicht:	London Nature Publishing Group UK 12.09.2022 Nature Publishing Group Nature Portfolio
Schlagworte:	140/133 140/146 147/135 147/137 147/143 639/638/92/173 639/925/357/354 639/925/357/995 639/925/357/997 Catalysis Depletion Electron transfer Electrons Engineering Enzymes Ferric ions Ferric oxide Ferrous ions Humanities and Social Sciences Ion migration Ions Iron oxides Iron phosphates Laboratories Lithium multidisciplinary Nanoparticles Oxidation Peroxidase Phase transitions Science Science (multidisciplinary)
ISSN:	2041-1723, 2041-1723
Online-Zugang:	Volltext
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Abstract	As pioneering Fe 3 O 4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe 2+ -induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe 2+ within Fe 3 O 4 can transfer electrons to the surface via the Fe 2+ -O-Fe 3+ chain, regenerating the surface Fe 2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe 3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe 3 O 4 nanozymes suffer the phase transformation to γ-Fe 2 O 3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes. The mechanism of peroxidase-like Fe 3 O 4 nanozymes remains elusive. Here, the authors show the electron transfer mechanism of Fe(II) ions to regenerate surface Fe(II) and the related phase transformation and depletion of activity.
AbstractList	As pioneering Fe3O4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe2+-induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe2+ within Fe3O4 can transfer electrons to the surface via the Fe2+-O-Fe3+ chain, regenerating the surface Fe2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe3O4 nanozymes suffer the phase transformation to γ-Fe2O3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes.As pioneering Fe3O4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe2+-induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe2+ within Fe3O4 can transfer electrons to the surface via the Fe2+-O-Fe3+ chain, regenerating the surface Fe2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe3O4 nanozymes suffer the phase transformation to γ-Fe2O3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes. As pioneering Fe 3 O 4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe 2+ -induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe 2+ within Fe 3 O 4 can transfer electrons to the surface via the Fe 2+ -O-Fe 3+ chain, regenerating the surface Fe 2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe 3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe 3 O 4 nanozymes suffer the phase transformation to γ-Fe 2 O 3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes. As pioneering Fe3O4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe2+-induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe2+ within Fe3O4 can transfer electrons to the surface via the Fe2+-O-Fe3+ chain, regenerating the surface Fe2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe3O4 nanozymes suffer the phase transformation to γ-Fe2O3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes. The mechanism of peroxidase-like Fe3O4 nanozymes remains elusive. Here, the authors show the electron transfer mechanism of Fe(II) ions to regenerate surface Fe(II) and the related phase transformation and depletion of activity. The mechanism of peroxidase-like Fe3O4 nanozymes remains elusive. Here, the authors show the electron transfer mechanism of Fe(II) ions to regenerate surface Fe(II) and the related phase transformation and depletion of activity. As pioneering Fe 3 O 4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe 2+ -induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe 2+ within Fe 3 O 4 can transfer electrons to the surface via the Fe 2+ -O-Fe 3+ chain, regenerating the surface Fe 2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe 3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe 3 O 4 nanozymes suffer the phase transformation to γ-Fe 2 O 3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes. The mechanism of peroxidase-like Fe 3 O 4 nanozymes remains elusive. Here, the authors show the electron transfer mechanism of Fe(II) ions to regenerate surface Fe(II) and the related phase transformation and depletion of activity.
ArticleNumber	5365
Author	Cheng, Wenlong Kong, Fei Che, Renchao Zhang, Yu Dong, Jian Dong, Haijiao Du, Wei Ma, Ming Gu, Ning
Author_xml	– sequence: 1 givenname: Haijiao orcidid: 0000-0001-8568-2757 surname: Dong fullname: Dong, Haijiao organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University, Jiangsu Key Laboratory for Biomaterials and Devices, School of Biological Science and Medical Engineering, Southeast University – sequence: 2 givenname: Wei orcidid: 0000-0002-9962-6630 surname: Du fullname: Du, Wei organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University, Jiangsu Key Laboratory for Biomaterials and Devices, School of Biological Science and Medical Engineering, Southeast University – sequence: 3 givenname: Jian surname: Dong fullname: Dong, Jian organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University – sequence: 4 givenname: Renchao orcidid: 0000-0002-6583-7114 surname: Che fullname: Che, Renchao organization: Laboratory of Advanced Materials, Fudan University, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Fudan University, Department of Materials Science, Fudan University – sequence: 5 givenname: Fei surname: Kong fullname: Kong, Fei organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University, Jiangsu Key Laboratory for Biomaterials and Devices, School of Biological Science and Medical Engineering, Southeast University – sequence: 6 givenname: Wenlong orcidid: 0000-0002-2346-4970 surname: Cheng fullname: Cheng, Wenlong organization: Department of Chemical Engineering, Faculty of Engineering, Monash University, The Melbourne Centre for Nanofabrication – sequence: 7 givenname: Ming orcidid: 0000-0001-5324-4082 surname: Ma fullname: Ma, Ming email: maming@seu.edu.cn organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University, Jiangsu Key Laboratory for Biomaterials and Devices, School of Biological Science and Medical Engineering, Southeast University – sequence: 8 givenname: Ning orcidid: 0000-0003-0047-337X surname: Gu fullname: Gu, Ning email: guning@seu.edu.cn organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University, Jiangsu Key Laboratory for Biomaterials and Devices, School of Biological Science and Medical Engineering, Southeast University – sequence: 9 givenname: Yu orcidid: 0000-0002-0228-7979 surname: Zhang fullname: Zhang, Yu email: zhangyu@seu.edu.cn organization: State Key Laboratory of Bioelectronics, School of Biological Science and Medical Engineering, Southeast University, Jiangsu Key Laboratory for Biomaterials and Devices, School of Biological Science and Medical Engineering, Southeast University
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Snippet	As pioneering Fe 3 O 4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe 2+... As pioneering Fe3O4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface... The mechanism of peroxidase-like Fe3O4 nanozymes remains elusive. Here, the authors show the electron transfer mechanism of Fe(II) ions to regenerate surface...
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SubjectTerms	140/133 140/146 147/135 147/137 147/143 639/638/92/173 639/925/357/354 639/925/357/995 639/925/357/997 Catalysis Depletion Electron transfer Electrons Engineering Enzymes Ferric ions Ferric oxide Ferrous ions Humanities and Social Sciences Ion migration Ions Iron oxides Iron phosphates Laboratories Lithium multidisciplinary Nanoparticles Oxidation Peroxidase Phase transitions Science Science (multidisciplinary)
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Title	Depletable peroxidase-like activity of Fe3O4 nanozymes accompanied with separate migration of electrons and iron ions
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