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1.
Dalton Trans ; 52(46): 17524-17537, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37961750

RESUMO

Highly active Keggin-type silicotungstic acid (SiW12) with oxygen vacancy (Ov) defects was encapsulated into the magnetic floral N-doped carbon microspheres (γ-Fe2O3@NC-300) through the facile one-step air pyrolysis of the precursor comprising core-shell Fe3O4@polydopamine (Fe3O4@PDA) and SiW12 to prepare γ-Fe2O3@NC@SiW12-300. The fabricated catalysts were systematically characterized and subsequently employed for the oxidation desulfurization (ODS) of the model fuel. The magnetic floral γ-Fe2O3@NC@SiW12-300 catalyst exhibited nearly perfect catalytic activity, which under mild conditions could remove 100% amount of 4000 ppm DBT in model fuel within 20 min (0.03 g catalysts and n(H2O2)/n(S) of 2). The catalyst activity is mainly attributed to the high activity SiW12 with the Ov defect and its outstanding dispersibility in γ-Fe2O3@NC, along with the high number of exposed active sites. A selected catalyst, γ-Fe2O3@NC@SiW12-300, showed a noticeable turnover frequency (TOF) (110.07 h-1) and lower activation energy (38.79 kJ mol-1) in oxidative desulfurization (ODS) with good recyclability. HO˙ radical was found to be the active species involved in ODS as confirmed by the EPR and scavenger experiments. Additionally, the fabricated catalyst can be conveniently separated and recycled within an externally applied magnetic field.

2.
RSC Adv ; 13(21): 14554-14564, 2023 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-37188247

RESUMO

An activated carbon-supported Cu/ZnO catalyst (CCZ-AE-ox) was successfully obtained by the ammonia evaporation method for the hydrogenation of carbon dioxide to methanol, and the surface properties of the catalyst post-calcination and reduction were investigated. Activated carbon facilitated the increased dispersion of the loaded metals, which promote the CO2 space-time yield (STY) of methanol and turnover frequency (TOF) on the active sites. Furthermore, the factors affecting the catalyst in the hydrogenation of CO2 to methanol were in-depth investigated. The larger surface area and higher CO2 adsorption capacity are found to make possible the main attributions of the superior activity of the CCZ-AE-ox catalyst.

3.
Dalton Trans ; 51(47): 18059-18067, 2022 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-36373745

RESUMO

The urea oxidation reaction (UOR), which possesses a low theoretical potential and superior kinetics, is an attractive substitute for the anodic oxygen evolution reaction (OER) in overall water splitting; however, the implementation of hydrogen production in overall urea splitting is impeded by the deficiency of highly efficient, durable and cost-effective catalysts. Herein, we fabricated an Ni2P-MoP2 heterostructure with a hierarchical structure grown on carbon paper (Ni-Mo-P/CP), which exhibited robust activity and outstanding durability for the electrocatalytic oxidation of urea. The Ni-Mo-P/CP catalyst possessed an ultralow potential of 1.39 V to obtain the current density of 100 mA cm-2, small Tafel slope (27 mV dec-1) and long-term durability with almost no decay within 15 h. The experimental characterization revealed that the optimized electronic structure and the synergistic effect of abundant exposed active sites in the Ni-Mo-P/CP catalyst contribute to the efficient UOR catalytic activity. This work enriches the candidate catalysts for the UOR and promotes the industrial development of hydrogen production.

4.
Small ; 17(10): e2005752, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33544971

RESUMO

Aromatic imides are a class of attractive organic materials with inherently electroactive groups and large π electron-deficient scaffolds, which hold potential as electrode materials for organic secondary batteries (OSBs). However, the undecorated aromatic imides are usually plagued by low capacity, high solubility in electrolyte, and poor electronic/ionic conductivity. Molecular engineering has been demonstrated to be an effective strategy to address unsatisfying characteristics of the aromatic imides, thereby expanding their scope for applications in OSBs. In this review, the recent research progress in modulation of the capacity, dissolution, and electronic/ionic conductivity of aromatic imides for organic lithium batteries, organic sodium batteries, and redox flow batteries are summarized. In addition, the challenge and prospective of aromatic imides in organic secondary battery applications are also discussed.

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