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1.
Inorg Chem ; 63(9): 4214-4223, 2024 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-38436239

RESUMEN

The reductive transformation of Cr(VI) into Cr(III) mediated by formic acid with efficient, stable, and cost-effective catalysts is a promising strategy for remediating Cr(VI) contamination. Herein, we report the facile construction of uniform Co@NC nanosheet-assembled microflowers for the reduction of Cr(VI). Both experimental results and density functional theory (DFT) calculations reveal the vital role of the intensive interfacial electronic interaction between Co nanoparticles and the N-doped carbon layer in facilitating the anchoring and dispersion of Co nanoparticles within the carbon framework. The interfacial electron transfer from Co to NC contributes to the interaction with Cr2O72- ions, promoting the subsequent H-transfer reaction. A Langmuir-Hinshelwood kinetic model has been established for the Cr(VI) reduction catalyzed by the CNCF2 (pyrolyzed at 700 °C), which shows a superior reaction performance. This study provides a facile strategy to delicately design well-assembled heterostructures with rich interfaces and strong interfacial interactions for a series of applications in environmental/thermal catalysis.

2.
J Colloid Interface Sci ; 606(Pt 2): 1758-1766, 2022 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-34500173

RESUMEN

Metal-free catalysts with environmental friendless, cost-competitiveness and less susceptibility to leaching and poisoning over metal-based catalysts, have revolutionized in the catalysis domain. In this respect, we herein report the first application of cheap and abundant pumpkin-derived N-doped porous carbon for the reduction of 2-methyl-4-nitrophenol assisted by NaBH4. The obtained catalyst is cost-competitive, efficient and robust, with an attractive mass-normalized rate constant of 4.73 s-1 g-1 and good recycling performance. Systematical analyses demonstrate that the 2-methyl-4-nitrophenol reduction reaction catalyzed by the N-doped carbon proceeds through the Langmuir-Hinshelwood kinetics and the performance enhancement benefits from the strong adsorption and activation of the substrates induced by the electronic modulation in the carbon framework via N-doping. This study opens up new avenues for the high-value use of pumpkin as well as the development of metal-free strategy in more catalytic applications.


Asunto(s)
Carbono , Cucurbita , Nitrógeno , Nitrofenoles , Porosidad
3.
J Colloid Interface Sci ; 585: 61-71, 2021 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-33279707

RESUMEN

The direct oxidation of styrene into high-value chemicals under mild reaction conditions remains a great challenge in both academia and industry. Herein, we report a successful electronic structure modulation of intrinsic NiO sheets via Mn-doping towards the oxidation of styrene. By doping NiO with only a small content of Mn (Mn/Ni atomic ratio of 0.030), a 75.0% yield of STO can be achieved under the optimized reaction conditions, which is 2.13 times higher than that of the pure NiO. In addition, the catalyst exhibits robust stability and good recycling performance. The performance enhancement originates from the synergistic effect regarding the abundant Ni(II) species, the rich oxygen vacancy sites and the large amount of surface redox centers. This work provides new findings of the elemental-doping-induced multifunctionality in designing powerful catalysts for the efficient and selective oxidation of styrene and beyond.

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