High oxidase-mimic activity of Fe nanoparticles embedded in an N-rich porous carbon and their application for sensing of dopamine

Chen, Qiumeng; Liang, Chunhong; Zhang, Xiaodan; Huang, Yuming

doi:10.1016/j.talanta.2018.02.032

Cited by 81 publications

(39 citation statements)

References 51 publications

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“…The peaks at 707.1 and 711.5 eV demonstrate the presence of Fe–N x species . Besides, the peaks at 708.2 eV (Fe 2p 3/2 ) and 720.4 eV (Fe 2p 1/2 ) indicate the existence of Fe 0 , which is in accord with XRD results. Since XPS can only detect the chemical states of material surface, the peaks of metallic iron with external coverage of Fe 4 N or iron oxide are relatively weak, which can be illustrated by the TEM image (Figure S5, Supporting Information).…”

Section: Resultssupporting

confidence: 86%

“…Fe–N x structure in the carbon shell is regarded as an active site for ORR in FFPC/N‐doped porous carbon nanofibers (NPCNFs). The high‐resolution N 1s spectrum could be deconvoluted into five different peaks at 398.4, 398.9, 399.9, 400.9, and 402.8 eV, which were attributed to the overlap of pyridinic N, Fe–N, pyrrolic N, graphitic‐N, and N‐oxide, respectively . The related high‐resolution C 1s spectrum is convoluted into two strong peaks at 284.…”

Section: Resultsmentioning

confidence: 98%

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Yolk–Shell Fe/Fe₄N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Jiao

Chen

You

et al. 2019

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A yolk-shell Fe/Fe 4 N@Pd/C (FFPC) nanocomposite is synthesized successfully by two facile steps: interfacial polymerization and annealing treatment. The concentration of Pd 2+ is the key factor for the density of Pd nanoparticles (Pd NPs) embedded in the carbon shells, which plays a role in the oxygen reduction reaction (ORR) and surface-enhanced Raman scattering (SERS) properties. The ORR and SERS performances of FFPC nanocomposites under different concentrations of PdCl 2 are investigated. The optimal ORR performance exhibits that onset potential and tafel slope can reach 0.937 V (vs reversible hydrogen electrode (RHE)) and 74 mV dec −1 , respectively, which is attributed to the synergistic effects of good electrical conductivity, large electrochemically active areas, and strong interfacial charge polarization. Off-axis electron holography reveals that interfacial charge polarization could facilitate the ORR of Pd NPs and defective carbon simultaneously and the shell with low density of Pd NPs is easier to form strong interfacial charge polarization. Moreover, FFPC-3 with maximum EF of 2.3 × 10 5 results from more hot-spots, local positive charge centers to attract rhodamine 6G molecules, and magnetic cores. This work not only offers a recyclable multifunctional nanocomposite with excellent performance, but also has instructional implications for interfacial engineering for electrocatalysts design.Multifunctional Nanocomposites www.advancedsciencenews.com

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Section: Resultssupporting

confidence: 86%

Section: Resultsmentioning

confidence: 98%

Yolk–Shell Fe/Fe₄N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Jiao

Chen

You

et al. 2019

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“…However, the precise mechanism of this catalytic activation of atmospheric oxygen is still under debate. Chen et al [3,19] The hydrogen peroxide reacting with the Fe 2+ /Fe 3+ in the Fe-N x -C structure can generate superoxide radicals. H 2 O 2 can also react with the Fe-N x centers and produce • OH by a Fenton-like reaction.…”

Section: Discussionmentioning

confidence: 99%

“…ROS may be generated abiotically when hydrogen peroxide reacts with Fe-containing nanomaterials leading to the production of superoxide radicals ( • O 2 − ), hydroxyl radicals ( • OH), or singlet oxygen species ( 1 O 2 ). This process is similar to the activity of peroxidases, which catalyze the reaction of H 2 O 2 with organic substrates via ROS generation [3][4][5][6]. For these reasons, the possible antibiotic properties of the nanozymes as well as their implementation for nanotechnology as the ROS determination agents have been studied intensively over the last several years.…”

Section: Introductionmentioning

confidence: 98%

“…with oxygen leading to • O 2 − generation [19]. As a result, the Fe-doped carbons are able to mimic oxidase activity by producing H 2 O 2 directly from atmospheric oxygen, yet simultaneously they can act as peroxidases catalyzing the hydrogen peroxide reduction [3][4][5][6]. Not only heteroatom-doped carbons, but a variety of Fe-containing materials and structures (e.g., F 2 O 3 , Fe 3 S 4 , etc.…”

Section: Introductionmentioning

confidence: 99%

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Interactions of Fe–N–S Co-Doped Porous Carbons with Bacteria: Sorption Effect and Enzyme-Like Properties

et al. 2020

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Carbon-based (nano)materials doped with transition metals, nitrogen and other heteroatoms are considered active heterogeneous catalysts in a wide range of chemical processes. Recently they have been scrutinized as artificial enzymes since they can catalyze proton-coupled electron transfer reactions vital for living organisms. Herein, interactions between Gram-positive and Gram-negative bacteria and either metal-free N and/or S doped or metal containing Fe−N−S co-doped porous carbons are studied. The Fe- and N-co-doped porous carbons (Fe−N−C) exhibit enhanced affinity toward bacteria as they show the highest adsorption capacity. Fe−N−C materials also show the strongest influence on the bacteria viability with visible toxic effect. Both types of bacteria studied reacted to the presence of Fe-doped carbons in a similar manner, showing a decrease in dehydrogenases activity in comparison to controls. The N-coordinated iron-doped carbons (Fe−N−C) may exhibit oxidase/peroxidase-like activity and activate O2 dissolved in the solution and/or oxygen-containing species released by the bacteria (e.g., H2O2) to yield highly bactericidal reactive oxygen species. As Fe/N/ and/or S-doped carbon materials efficiently adsorb bacteria exhibiting simultaneously antibacterial properties, they can be applied, inter alia, as microbiological filters with enhanced biofouling resistance.

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A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers

et al. 2022

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MetalN-coordinated centers supported by carbonaceous substrates have emerged as promising artificial metalloenzymes (AMEs) to mimic the biocatalytic effects of their natural counterparts. However, the synthesis of well-defined AMEs that contain different atomic metalN centers but present similar physicochemical and coordination structures remains a substantial challenge. Here, 20 different types of AMEs with similar geometries and welldefined atomic metalN-coordinated centers are synthesized to compare and disclose the catalytic activities, substrate selectivities, kinetics, and reactive oxygen species (ROS) products. Their oxidase (OXD)-, peroxidase (POD)-, and halogen peroxidase (HPO)-mimetic catalytic behaviors are systematically explored. The Fe-AME shows the highest OXD-and HPO-mimetic activities compared to the other AMEs due to its high v max (0.927 × 10 −6 m s −1 ) and low K m (1.070 × 10 −3 m), while the Cu-AME displays the best POD-like performance. Furthermore, theoretical calculation reveals that the ROS-catalytic paths and activities are highly related to the electronic structures of the metal centers. Benefiting from its facile adsorption of H 2 O 2 molecule and lower energy barrier to generating •O 2 − , the Fe-AME displays higher ROS-catalytic performances than the Mn-AME. The engineered AMEs show not only remarkably high ROS-catalytic performances but also provide new guidance toward developing metalN-coordinated biocatalysts for broad application fields.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202200255.

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High oxidase-mimic activity of Fe nanoparticles embedded in an N-rich porous carbon and their application for sensing of dopamine

Cited by 81 publications

References 51 publications

Yolk–Shell Fe/Fe₄N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Yolk–Shell Fe/Fe₄N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Interactions of Fe–N–S Co-Doped Porous Carbons with Bacteria: Sorption Effect and Enzyme-Like Properties

A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers

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High oxidase-mimic activity of Fe nanoparticles embedded in an N-rich porous carbon and their application for sensing of dopamine

Cited by 81 publications

References 51 publications

Yolk–Shell Fe/Fe4N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Yolk–Shell Fe/Fe4N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Interactions of Fe–N–S Co-Doped Porous Carbons with Bacteria: Sorption Effect and Enzyme-Like Properties

A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers

Contact Info

Product

Resources

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Yolk–Shell Fe/Fe₄N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate

Yolk–Shell Fe/Fe₄N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate