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1.
Angew Chem Int Ed Engl ; : e202410413, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38973379

RESUMO

The catalytic activity of platinum for the CO oxidation depends on the interaction of electron donation and back-donation at the platinum center. Here we demonstrate that the platinum bromine nanoparticles with electron-rich properties on bromine bonded with sp-C in graphdiyne (PtBr NPs/Br-GDY), which is formed by bromine ligand and constitutes an electrocatalyst with a high CO-resistant for methanol oxidation reaction (MOR). The catalyst showed peak mass activity for MOR as high as 10.4 A mgPt-1, which is 20.8 times higher than the 20% Pt/C. The catalyst also showed robust long-term stability with slight current density decay after 100 hours at 35 mA cm-2. Structural characterization, experimental, and theoretical studies show that the electron donation from bromine makes the surface of platinum catalysts highly electron-rich, and can strengthen the adsorption of CO as well as enhance π back-donation of Pt to weaken the C-O bond to facilitate CO electrooxidation and enhance catalytic performance during MOR. The results highlight the importance of electron-rich structure among active sites in Pt-halogen catalysts and provide detailed insights into the new mechanism of CO electrooxidation to overcome CO poisoning at the Pt center on an orbital level.

2.
Angew Chem Int Ed Engl ; 62(40): e202308968, 2023 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-37581223

RESUMO

Controlling the structure and properties of catalysts through atomic arrangement is the source of producing a new generation of advanced catalysts. A highly active and stable catalyst in catalytic reactions strongly depends on an ideal arrangement structure of metal atoms. We demonstrated that the introduction of the defect-rich structures, low coordination number (CN), and tensile strain in three-dimensional (3D) urchin-like palladium nanoparticles through chlorine bonded with sp-C in graphdiyne (Pd-UNs/Cl-GDY) can regulate the arrangement of metal atoms in the palladium nanoparticles to form a special structure. In situ Fourier infrared spectroscopy (FTIR) and theoretical calculation results show that Pd-UNs/Cl-GDY catalyst is beneficial to the oxidation and removal of CO intermediates. The Pd-UNs/Cl-GDY for methanol oxidation reaction (MOR) that display high current density (363.6 mA cm-2 ) and mass activity (3.6 A mgPd -1 ), 12.0 and 10.9 times higher than Pd nanoparticles, respectively. The Pd-UNs/Cl-GDY catalyst also exhibited robust stability with still retained 95 % activity after 2000 cycles. A defects libraries of the face-centered cubic and hexagonal close-packed crystal catalysts (FH-NPs) were synthesized by introducing chlorine in graphdiyne. Such defect-rich structures, low CN, and tensile strain tailoring methods have opened up a new way for the catalytic reaction of MOR.

3.
J Colloid Interface Sci ; 661: 840-852, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38330656

RESUMO

Magnetic carbon-based catalysts with environmental friendliness have exhibited prominent effects on advanced oxidation processes. Herein, a multi-level FeCo/N-doped carbon nanosheet (FeCo/CNS) was synthesized by facile impregnation iron-cobalt salt onto cotton and followed by confined pyrolysis. We identified excellent advantages of the modified FeCo/CNS materials: (i) The convenience of the synthesis method and (ii) The dual effect of sterilization and contaminant degradation achieved through the FeCo/CNS-activated Peroxymonosulfate (PMS). The comparative experimental showed that FeCo/CNS could provide favorable catalytic performance, completely removing bisphenol A (BPA) and tetracycline (TC) within 5 min. Moreover, the potent sterilization properties against Staphylococcus aureus and Escherichia coli were also verified. Analysis of the degradation pathway confirmed the existence of intermediates, and toxicological research demonstrated that the toxicity of the degradation intermediates of BPA gradually decreased over time. Our research provided an excellent application of FeCo/CNS in PMS oxidation and sterilization inactivation.


Assuntos
Compostos Benzidrílicos , Carbono , Compostos de Ferro , Fenóis , Peróxidos , Ferro
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