High-spin surface FeIV = O synthesis with molecular oxygen and pyrite for selective methane oxidation

Nature-inspired high-spin Fe IV  = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡Fe II …Fe II ≡ sites on pyrite (FeS 2 ) mimicking soluble methane monooxygenase, we achieve O 2 -driven formation of high-spin (S = 2) surface Fe IV  = O species at room t...

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Published inNature communications Vol. 16; no. 1; pp. 7642 - 9
Main Authors Ling, Cancan, Li, Meiqi, Li, Hao, Liu, Xiufan, Guo, Furong, Liu, Yi, Zhang, Rui, Zhao, Jincai, Zhang, Lizhi
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 16.08.2025
Nature Publishing Group
Nature Portfolio
Subjects
639/638/224/685
639/638/77/884
639/638/77/885
639/638/77/887
Adsorption
Benchmarks
Chemical synthesis
Electrons
Energy
Geometry
Humanities and Social Sciences
Hydrogen peroxide
Intermediates
Iron
Iron sulfides
Ligands
Methane
Methane monooxygenase
multidisciplinary
Oxidation
Oxygen transfer
Pyrite
Room temperature
Science
Science (multidisciplinary)
Selectivity
Soluble methane monooxygenase
Sulfur
Symmetry
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Abstract Nature-inspired high-spin Fe IV  = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡Fe II …Fe II ≡ sites on pyrite (FeS 2 ) mimicking soluble methane monooxygenase, we achieve O 2 -driven formation of high-spin (S = 2) surface Fe IV  = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O 2 activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O − O bond cleavage. The resulting Fe IV  = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this configuration can efficiently convert CH 4 to CH 3 OH through an oxygen transfer reaction with a synthetic efficiency of TOF = 27.4 h −1 and selectivity of 87.0%, outperforming most ambient O 2 -driven benchmarks under comparable conditions and even surpassing many H 2 O 2 -mediated systems. This study offers a facile method to synthesize high-spin surface Fe IV  = O and highlights the importance of metal spin state tailoring on non-enzymatic methane activation. High-spin Fe(IV) = O sites efficiently activate methane but are challenging to synthesize. This study develops dual Fe(II) sites on FeS 2 , generating high-spin Fe(IV) = O from O 2 , achieving superior methane-to-methanol conversion under mild conditions.
AbstractList Nature-inspired high-spin Fe IV  = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡Fe II …Fe II ≡ sites on pyrite (FeS 2 ) mimicking soluble methane monooxygenase, we achieve O 2 -driven formation of high-spin (S = 2) surface Fe IV  = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O 2 activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O − O bond cleavage. The resulting Fe IV  = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this configuration can efficiently convert CH 4 to CH 3 OH through an oxygen transfer reaction with a synthetic efficiency of TOF = 27.4 h −1 and selectivity of 87.0%, outperforming most ambient O 2 -driven benchmarks under comparable conditions and even surpassing many H 2 O 2 -mediated systems. This study offers a facile method to synthesize high-spin surface Fe IV  = O and highlights the importance of metal spin state tailoring on non-enzymatic methane activation. High-spin Fe(IV) = O sites efficiently activate methane but are challenging to synthesize. This study develops dual Fe(II) sites on FeS 2 , generating high-spin Fe(IV) = O from O 2 , achieving superior methane-to-methanol conversion under mild conditions.
Nature-inspired high-spin FeIV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡FeII…FeII≡ sites on pyrite (FeS2) mimicking soluble methane monooxygenase, we achieve O2-driven formation of high-spin (S = 2) surface FeIV = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O2 activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O − O bond cleavage. The resulting FeIV = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this configuration can efficiently convert CH4 to CH3OH through an oxygen transfer reaction with a synthetic efficiency of TOF = 27.4 h−1 and selectivity of 87.0%, outperforming most ambient O2-driven benchmarks under comparable conditions and even surpassing many H2O2-mediated systems. This study offers a facile method to synthesize high-spin surface FeIV = O and highlights the importance of metal spin state tailoring on non-enzymatic methane activation.High-spin Fe(IV) = O sites efficiently activate methane but are challenging to synthesize. This study develops dual Fe(II) sites on FeS2, generating high-spin Fe(IV) = O from O2, achieving superior methane-to-methanol conversion under mild conditions.
Nature-inspired high-spin FeIV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡FeII…FeII≡ sites on pyrite (FeS2) mimicking soluble methane monooxygenase, we achieve O2-driven formation of high-spin (S = 2) surface FeIV = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O2 activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O - O bond cleavage. The resulting FeIV = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this configuration can efficiently convert CH4 to CH3OH through an oxygen transfer reaction with a synthetic efficiency of TOF = 27.4 h-1 and selectivity of 87.0%, outperforming most ambient O2-driven benchmarks under comparable conditions and even surpassing many H2O2-mediated systems. This study offers a facile method to synthesize high-spin surface FeIV = O and highlights the importance of metal spin state tailoring on non-enzymatic methane activation.Nature-inspired high-spin FeIV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡FeII…FeII≡ sites on pyrite (FeS2) mimicking soluble methane monooxygenase, we achieve O2-driven formation of high-spin (S = 2) surface FeIV = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O2 activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O - O bond cleavage. The resulting FeIV = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this configuration can efficiently convert CH4 to CH3OH through an oxygen transfer reaction with a synthetic efficiency of TOF = 27.4 h-1 and selectivity of 87.0%, outperforming most ambient O2-driven benchmarks under comparable conditions and even surpassing many H2O2-mediated systems. This study offers a facile method to synthesize high-spin surface FeIV = O and highlights the importance of metal spin state tailoring on non-enzymatic methane activation.
Abstract Nature-inspired high-spin FeIV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡FeII…FeII≡ sites on pyrite (FeS2) mimicking soluble methane monooxygenase, we achieve O2-driven formation of high-spin (S = 2) surface FeIV = O species at room temperature and pressure. Strategic removal of bridging S atoms creates active sites that facilitate O2 activation via transient ≡Fe-O-O-Fe≡ intermediates, promoting homolytic O − O bond cleavage. The resulting FeIV = O exhibits an asymmetrically distorted coordination environment that reduces the crystal field splitting and favors the occupation of higher energy d-orbitals with unpaired electrons. Impressively, this configuration can efficiently convert CH4 to CH3OH through an oxygen transfer reaction with a synthetic efficiency of TOF = 27.4 h−1 and selectivity of 87.0%, outperforming most ambient O2-driven benchmarks under comparable conditions and even surpassing many H2O2-mediated systems. This study offers a facile method to synthesize high-spin surface FeIV = O and highlights the importance of metal spin state tailoring on non-enzymatic methane activation.
ArticleNumber 7642
Author Ling, Cancan
Zhang, Lizhi
Liu, Xiufan
Guo, Furong
Zhao, Jincai
Li, Hao
Liu, Yi
Zhang, Rui
Li, Meiqi
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  email: zhanglizhi@sjtu.edu.cn
  organization: State Key Laboratory of Green Papermaking and Resource Recycling, National Observation and Research Station of Erhai Lake Ecosystem in Yunnan, Yunnan Dali Research Institute, School of Environmental Science and Engineering, Shanghai Jiao Tong University
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Snippet Nature-inspired high-spin Fe IV  = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡Fe II …Fe II ≡ sites on pyrite...
Nature-inspired high-spin FeIV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡FeII…FeII≡ sites on pyrite...
Abstract Nature-inspired high-spin FeIV = O generation enables efficient ambient methane oxidation. By engineering sulfur-bridged dual ≡FeII…FeII≡ sites on...
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SubjectTerms 639/638/224/685
639/638/77/884
639/638/77/885
639/638/77/887
Adsorption
Benchmarks
Chemical synthesis
Electrons
Energy
Geometry
Humanities and Social Sciences
Hydrogen peroxide
Intermediates
Iron
Iron sulfides
Ligands
Methane
Methane monooxygenase
multidisciplinary
Oxidation
Oxygen transfer
Pyrite
Room temperature
Science
Science (multidisciplinary)
Selectivity
Soluble methane monooxygenase
Sulfur
Symmetry
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Title High-spin surface FeIV = O synthesis with molecular oxygen and pyrite for selective methane oxidation
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