Porphyrin polymer-derived single-atom Fe assisted by Fe2O3 with oxygen vacancy for efficient oxygen reduction reaction

Ren, Jianwei; Yan, Wei; Li, Xue; Wang, Fuling; Xing, Qianli; Xiao, Zuoxu; Liu, Heyuan; Chen, Yanli; Li, Xiyou

doi:10.1016/j.apsusc.2022.153301

Cited by 19 publications

(2 citation statements)

References 51 publications

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“…The WT maps (Figure 2i) reveal the same maximum intensity as FePc at ≈4.0 Å −1 originating from Fe─N bonding, which is different from the WT maximum intensity at 4.9 Å −1 originating from Fe─O bonding in the Fe 2 O 3 . [24] This proves that the single Fe atoms in Pt/HFe SA -HCS exist in Fe─N coordination form. The corresponding EXAFS fitting curves of Pt/HFe SA -HCS in the R space of the Fe K-edge also matched well with experimental results (Figure S17 and Table S3, Supporting Information), confirming that the single Fe atom was coordinated to ≈4 N atoms in Pt/HFe SA -HCS.…”

Section: Electronic Structure and Chemical Statesmentioning

confidence: 69%

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N₄ for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Yan,

Xing,

Ren

et al. 2023

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Decorating platinum (Pt) with a single atom offers a promising approach to tailoring their catalytic activity. In this study, for the first time, an innovative assistive active sites (AAS) strategy is proposed to construct high–loading (3.46wt.%) single Fe─N4 as AAS, which are further hybridized with small Pt nanoparticles to enhance both oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activities. For ORR, the target catalyst (Pt/HFeSA–HCS) exhibits a higher mass activity (MA) of 0.98 A mgPt−1 and specific activity (SA) of 1.39 mA cmPt−2 at 0.90 V versus RHE. As for MOR, Pt/HFeSA–HCS shows exceptional MA (3.21 A mgPt−1) and SA (4.27 mA cmPt−2) at peak values, surpassing commercial Pt/C by 15.3 and 11.5 times, respectively. The underlying mechanism behind this AAS strategy is to find that in MOR, Fe─N4 promotes water dissociation, generating more *OH to accelerate the conversion of *CO to CO2. Meanwhile, in ORR, Fe─N4 acts as a competitor to adsorb *OH, weakening Pt─OH bonding and facilitating desorption of *OH on the Pt surface. Constructing AAS that can enhance dual functionality simultaneously can be seen as a successful “kill two birds with one stone” strategy.

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Section: Electronic Structure and Chemical Statesmentioning

confidence: 69%

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N₄ for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Yan,

Xing,

Ren

et al. 2023

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“…32,33 Meanwhile, the selected organic building block porphyrins with a delocalized p-electron system provide a rigid and planar structure, large surface area, and high-density activity, which facilitate intramolecular and intermolecular charge transfer on the polymer backbones. 34,35 For above considerations, three CMPs with different asymmetry degrees were prepared by using 4-[10,15,20-tris(4-aminophenyl)-21,24-dihydroporphyrin-5-yl] aniline as an organic linker, and uorene (BB), indenothiophene (BT), and boron nitrogen-containing units (BN) as building units via Buchwald Hartwig coupling reactions, [36][37][38] which were named PPA-BB, PPA-BT, and PPA-BN, respectively. As Fig.…”

Section: Resultsmentioning

confidence: 99%

Porphyrin-containing conjugated microporous polymers with gradient asymmetric design for efficient oxygen reduction

Zheng,

Wang,

Wang

et al. 2024

J. Mater. Chem. A

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Employing Noble Metal–Porphyrins to Engineer Robust and Highly Active Single‐Atom Nanozymes for Targeted Catalytic Therapy in Nasopharyngeal Carcinoma

Wang,

Gao

et al. 2023

Advanced Materials

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Single‐atom nanozymes (SANzymes) emerge as promising alternatives to conventional enzymes. However, chemical instability limits their application. Here, a systematic synthesis of highly active and stable SANzymes is presented by leveraging noble metal–porphyrins. Four noble metal–porphyrins are successfully synthesized to mimic the active site of natural peroxidases through atomic metal–N coordination anchored to the porphyrin center. These noble metal–porphyrins are integrated into a stable and biocompatible Zr‐based metal–organic framework (MxP, x denoting Ir, Ru, Pt, and Pd). Among these, MIrP demonstrates superior peroxidase‐like activity (685.61 U mg−1), catalytic efficiency, and selectivity compared to horseradish peroxidase (267.71 U mg−1). Mechanistic investigations unveil heightened catalytic activity of MIrP arises from its robust H2O2 adsorption capacity, unique rate‐determining step, and low energy threshold. Crucially, MIrP exhibits remarkable chemical stability under both room temperature and high H2O2 concentrations. Further, through modification with (−)‐Epigallocatechin‐3‐Gallate, a natural ligand for Epstein–Barr virus (EBV)‐encoded latent membrane protein 1, targeted SANzyme (MIrPHE) tailored for EBV‐associated nasopharyngeal carcinoma is engineered. This study not only presents an innovative strategy for augmenting the catalytic activity and chemical stability of SANzymes but also highlights the substantial potential of MIrP as a potent nanomedicine for targeted catalytic tumor therapy.

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Porphyrin polymer-derived single-atom Fe assisted by Fe2O3 with oxygen vacancy for efficient oxygen reduction reaction

Cited by 19 publications

References 51 publications

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N₄ for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N₄ for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Porphyrin-containing conjugated microporous polymers with gradient asymmetric design for efficient oxygen reduction

Employing Noble Metal–Porphyrins to Engineer Robust and Highly Active Single‐Atom Nanozymes for Targeted Catalytic Therapy in Nasopharyngeal Carcinoma

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Porphyrin polymer-derived single-atom Fe assisted by Fe2O3 with oxygen vacancy for efficient oxygen reduction reaction

Cited by 19 publications

References 51 publications

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N4 for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N4 for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Porphyrin-containing conjugated microporous polymers with gradient asymmetric design for efficient oxygen reduction

Employing Noble Metal–Porphyrins to Engineer Robust and Highly Active Single‐Atom Nanozymes for Targeted Catalytic Therapy in Nasopharyngeal Carcinoma

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Product

Resources

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Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N₄ for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy

Enhanced Activity of Small Pt Nanoparticles Decorated with High‐Loading Single Fe─N₄ for Methanol Oxidation and Oxygen Reduction via the Assistive Active Sites Strategy