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1.
Beilstein J Org Chem ; 20: 1906-1913, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-39135660

RESUMO

A novel facile approach to N-arylpyridoindazolium salts is proposed, based on direct oxidation of the ortho-pyridine substituted diarylamines, either using bis(trifluoroacetoxy)iodobenzene as an oxidant, or electrochemically, via potentiostatic oxidation. Electrochemical synthesis occurs under mild conditions; no chemical reagents are required except electric current. Both approaches can be considered as a late-stage functionalization; easily available ortho-pyridyl-substituted diarylamines are used as the precursors.

2.
Environ Technol ; : 1-10, 2024 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-39150864

RESUMO

This article explores the benefits of electrochemical oxidation in pulsed mode, using potential, current, and power pulses. While potential and current pulse electrochemical technology has been previously studied for wastewater treatment, no study has included power pulses until now. The objective of this work is to highlight the advantages of power pulses by applying this pulse type to the electrochemical oxidation of a probe molecule, alachlor. For this aim, the influence of operating parameters and the comparison of the different pulse modes were investigated and compared to the results obtained with the electrochemical oxidation of alachlor in continuous mode. The study shows that the best results were obtained with the power pulse electrochemical oxidation with 100% alachlor degradation after 180 min and a mineralisation yield of 38.3% after 240 min. These results were better than those reported in the literature for treatments with continuous current input using platinum electrodes. This new technique could be an effective and efficient way to treat contaminated water and reduce the pressure on freshwater reserves.

3.
Chemistry ; 30(54): e202402220, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39012680

RESUMO

The advancement in electrochemical techniques has unlocked a new path for achieving unprecedented oxidations and reductions of aryl radical precursors in a controlled and selective manner. This approach facilitates the construction of aromatic carbon-carbon and carbon-heteroatom bonds. In light of the green merits and the growing importance of this technique in aryl radical chemistry, this review aims to provide an overview of the recent advance in the electrochemical generation of aryl radicals organized by the aryl radical precursor type, with a focus on the substrate scope, limitation, and underlying mechanism, thereby inspiring future work on electrochemical aryl radical generation.

4.
Angew Chem Int Ed Engl ; : e202407207, 2024 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-39075778

RESUMO

This Minireview examines a selection of case studies that showcase distinctive and enabling electrochemical approaches that have allowed for the generation and reaction of carbocation intermediates under mild conditions. Particular emphasis is placed on the progress that has been made in this area of organic synthesis and polymer chemistry over the past decade.

5.
Environ Sci Pollut Res Int ; 31(34): 46910-46948, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38995339

RESUMO

The principle of Fenton reagent is to produce ·OH by mixing H2O2 and Fe2+ to realize the oxidation of organic pollutants, although Fenton reagent has the advantages of non-toxicity and short reaction time, but there are its related defects. The Fenton-like technology has been widely studied because of its various forms and better results than the traditional Fenton technology in terms of pollutant degradation efficiency. This paper reviews the electro-Fenton technology among the Fenton-like technologies and provides an overview of the homogeneous electro-Fenton. It also focuses on summarizing the effects of factors such as H2O2, reactant concentration, reactor volume and electrode quality, reaction time and voltage (potential) on the efficiency of electro-Fenton process. It is shown that appropriate enhancement of H2O2 concentration, voltage (potential) and reaction volume can help to improve the process efficiency; the process efficiency also can be improved by increasing the reaction time and electrode quality. Feeding modes of H2O2 have different effects on process efficiency. Finally, a considerable number of experimental studies have shown that the combination of electro-Fenton with ultrasound, anodic oxidation and electrocoagulation technologies is superior to the single electro-Fenton process in terms of pollutant degradation.


Assuntos
Peróxido de Hidrogênio , Ferro , Peróxido de Hidrogênio/química , Ferro/química , Oxirredução , Técnicas Eletroquímicas
6.
Environ Sci Pollut Res Int ; 31(27): 39663-39677, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38831146

RESUMO

The mixed wastewater generated by anodic oxidation coating facilities contains high levels of various contaminants, including iron, aluminum, conductivity, chemical oxygen demand (COD), and sulfate. In this study, the effectiveness of the membrane distillation (MD) process using polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF) membranes was investigated to treat mixed wastewater from an anodized coating factory. The results indicate that both hydrophobic membranes effectively removed targeted contaminants. However, the PTFE membrane achieved higher removal efficiencies, with over 99% removal of sulfate, conductivity, iron, and aluminum, 85.7% of COD, and 86% of total organic carbon (TOC). In contrast, the PVDF membrane exhibited a significant decline in removal efficiency as the temperature increased and performed well only at lower feed temperatures. The PTFE membranes outperformed the PVDF membranes in treating chemically intensive anodic oxidation wastewaters. This superiority can be attributed to the PTFE membrane's morphology and structure, which are less influenced by feed water temperature and chemicals. Additionally, its slippery surface imparts anti-adhesion properties, effectively preventing membrane fouling, and maintaining the treated water quality and flux for longer operation time.


Assuntos
Destilação , Membranas Artificiais , Oxirredução , Politetrafluoretileno , Polivinil , Águas Residuárias , Águas Residuárias/química , Politetrafluoretileno/química , Polivinil/química , Eliminação de Resíduos Líquidos/métodos , Purificação da Água/métodos , Poluentes Químicos da Água , Polímeros de Fluorcarboneto
7.
Environ Technol ; : 1-7, 2024 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-38875359

RESUMO

Using oil recovery wastewater as the target material, the degradation of organic matter in oilfield wastewater was studied in an anodic oxidation system using Ti/Ru-Ir oxide-coated anode and 0.7mMNa2SO4 as the electrolyte. The TOC of the wastewater was 210 mg/L at the beginning of the electrolysis in the electrolysis system, and it decreased from 210 to 93.6 mg/L after 50 min of electrolysis. Under the action of this system, sulfate was oxidized to persulfate, and the apparent concentration of persulfate was 15.02 mM, oxidation and degradation of organic matter in wastewater by the action of newly generated persulfate.. Afterwards, NaOH and Fe2(SO4)3 were added to the electrolyzed wastewater, and the TOC in the wastewater was further reduced to 25.1 mg/L due to the coagulation effect of the newly generated Fe(OH)3 precipitate. The TOC removal rate of the wastewater treated by this process reached 88.0%, which meets the discharge requirements. At the same time, the derived persulfate oxidized Fe(OH)3 to generate a green substance, which was identified as Na2FeO3 by IR, UV, and XRD analyses. Na2FeO3 served as a highly effective water-purifying agent, demonstrating superior performance when compared to FeO42-. The method reported in this study not only provides a strategy for waste resource recycling but also offers the potential for mass production of ferrate (IV).

8.
ACS Appl Mater Interfaces ; 16(21): 27627-27639, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38766902

RESUMO

Ultrawide-spectra-compatible camouflage materials are imperative for military science and national security due to the continuous advancement of various sophisticated multispectral detectors. However, ultrawide spectra camouflage still has challenges, as the spectral requirements for different bands are disparate and even conflicting. This work demonstrates an ultrawide spectra camouflage material compatible with visible (VIS, 400-800 nm), infrared (IR, 3-5 and 8-14 µm), and microwave (S-Ku bands, 2-12 GHz). The carbon nanotubes adsorbed on porous anodic alumina/aluminum flake powder (CNTs@PAA/AFP) material for ultrawide spectra camouflage is composed of bioinspired porous alumina surface layers for low visible reflection and aluminum flake powder substrate for low infrared emissivity, while the surface of the porous alumina layers is loaded with carbon nanotubes for microwave absorption. Compared with previous low-emissivity materials, CNTs@PAA/AFP has omnidirectional low reflectance (Ravg = 0.29) and high gray scale (72%) in the visible band. Further, it exhibits low emissivity (ε3-5µm = 0.15 and ε8-14µm = 0.18) in the dual infrared atmospheric window, which reduces the infrared lock-on range by 59.6%/49.8% in the mid/far-infrared band at high temperatures (573 K). The infrared camouflage performance calculated from the radiation temperature of CNTs@PAA/AFP coatings is enhanced to over 65%, which is at least 4 times greater than that of its substrate. In addition, the CNTs@PAA/AFP coating achieves high microwave absorption (RLmin = -42.46 dB) and an effective absorption bandwidth (EAB = 7.43 GHz) in the microwave band (S-Ku bands) due to the enhancement of interfacial polarization and conductive losses. This study may introduce new insight and feasible methods for multispectral manipulation, electromagnetic signal processing, and thermal management via bioinspired structural design and fabrication.

9.
ChemSusChem ; 17(9): e202301691, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38192246

RESUMO

Methyl formate (MF) is one of the most important chemical commodities, which has a wide range of applications. Due to environmental friendliness, mild reaction conditions, and easy operations, electrosynthesis of MF has garnered increasing attention in recent years. In this work, we reported an electrosynthesis route toward MF in a halide-containing methanol solution. The thorough mechanistic investigations point out that electrosynthesis of MF is accomplished by instant reaction between aldehyde from anodic methanol oxidation, and methoxy bromide (CH3OBr) that is in-situ generated by reaction of Br2 from anodic oxidation of Br- with methoxide (CH3O-) from cathodic reduction of methanol. This method features high atomic economy only producing valuable MF and hydrogen gas, and shows distinct advantages compared to the reported MF electrosynthesis methods. Even at 200 mA/cm2, the faradaic efficiency (FE) of MF remains consistently around 60 % at the anode while a 100 % FE hydrogen gas is produced at the cathode.

10.
ACS Appl Mater Interfaces ; 16(3): 3260-3269, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38221720

RESUMO

The anode stability is critical for efficient and reliable seawater electrolyzers. Herein, a NiFe-based film catalyst was prepared by anodic oxidation to serve as a model electrode, which exhibited a satisfactory oxygen evolution performance in simulated alkaline seawater (1 M KOH + 0.5 M NaCl) with an overpotential of 348 mV at 100 mA cm-2 and a long-term stability of over 100 h. After that, the effects of the current density and bulk pH of the electrolyte on its stability were evaluated. It was found that the electrode stability was sensitive to electrolysis conditions, failing at 20 mA cm-2 in 0.1 M KOH + 0.5 M NaCl but over 500 mA cm-2 in 0.5 M KOH + 0.5 M NaCl. The electrode dissolved, and some precipitates immediately formed at the region very close to the electrode surface during the electrolysis. This can be ascribed to the pH difference between the electrode/electrolyte interface and the bulk electrolyte under anodic polarization. In other words, the microzone acidification accelerates the corrosion of the electrode by Cl-, thus affecting the electrode stability. The operational performances of the electrode under different electrolysis conditions were classified to further analyze the degradation behavior, which resulted in three regions corresponding to the stable oxygen evolution, violent dissolution-precipitation, and complete passivation processes, respectively. Thereby increasing the bulk pH could alleviate the microzone acidification and improve the stability of the anode at high current densities. Overall, this study provides new insights into understanding the degradation mechanism of NiFe-based catalysts and offers electrolyte engineering strategies for the application of anodes.

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