Study on maximizing catalytic performance of cobalt(II) 5,10,15,20-tetrakis(4-pyridyl)porphyrin for cyclohexane oxidation

Yuan, Guang-Ping; Huang, Guan; Wei, Su-Juan

doi:10.1016/j.jiec.2019.04.028

Cited by 24 publications

(4 citation statements)

References 44 publications

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“…The Co 2p high-resolution spectrum is consistent with the N 1s region, exhibiting clear Co 2+ –N peaks at 781.7 (2p 3/2 ) and 796.6 eV (2p 1/2 ). , Co 3+ –N species peaks are observable at 786.3 and 802.0 eV at a relatively low intensity. The appearance of the higher valence state of cobalt ions on the surface of the CN-CoPor/C composite is consistent with a previous report …”

Section: Resultssupporting

confidence: 93%

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Promotion of Catalytic Oxygen Reduction Reactions: The Utility of Proton Management Substituents on Cobalt Porphyrins

et al. 2022

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Three ABAB-type cobalt meso-tetraarylporphyrins with fluorine (F-CoPor), acetic acid (AC-CoPor), and cyanoacetic acid (CN-CoPor) groups at the para-positions of phenyl rings at the 10,20-positions are synthesized and evaluated as catalysts for oxygen reduction reactions (ORRs). In density functional theory calculations, the frontier molecular orbitals of these complexes were found to be stabilized relative to model complexes with electron-withdrawing atoms or moieties on the meso-aryl rings. Electrochemical measurements suggest that electrodes with CN-CoPor (CN-CoPor/C) exhibit the most positive ORR potential values and the highest limiting current density in both acidic and alkali electrolytes, while the F-CoPor/C electrocatalyst exhibits extremely low ORR performance. The electron transfer numbers for the electrocatalysts are more than 3.0, indicating that a mixture of 2-and 4-electron transfer pathways occurs. The results demonstrate that coupling the hydrogen bonding properties and electron-withdrawing abilities through rational design of the substituent at the meso-position is an efficient way to modify the ORR performance.

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Section: Resultssupporting

confidence: 93%

“…The appearance of the higher valence state of cobalt ions on the surface of the CN-CoPor/C composite is consistent with a previous report. 33 2.2. ORR Performance of the Electrocatalysts.…”

Section: Structural Design Of the Cobalt Porphyrinsmentioning

confidence: 99%

Promotion of Catalytic Oxygen Reduction Reactions: The Utility of Proton Management Substituents on Cobalt Porphyrins

et al. 2022

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“… , This is consistent with the Co 2p scan, which shows two bands at 780.8 eV (2 p 3/2 ) and 796.5 eV (2 p 1/2 ) assigned to Co 2+ –N (Figure S7b). No clear proof for the existence of Co–O (779.7 eV) or Co 3+ –N (785.6 and 802.5 eV) is observed in CP1@C . − …”

Section: Results and Discussionmentioning

confidence: 96%

Enhanced Oxygen Reduction Reaction Performance Using Intermolecular Forces Coupled with More Exposed Molecular Orbitals of Triphenylamine in Co-porphyrin Electrocatalysts

Zhao

Shao

et al. 2020

ACS Appl. Mater. Interfaces

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Triphenylamine (TPA) has often been used as a building block to construct functional organic materials yet is rarely employed in oxygen reduction reaction (ORR) due to its strong electron-donating ability. This versatile segment bears a three-dimensional spatial structure whose effect has not been fully explored in catalytic systems. To this end, five symmetric cobalt porphyrins with carbazole and TPA derivatives have been synthesized and their ORR performance has been evaluated in acid medium. It was found that all compounds produced mainly hydrogen peroxide in oxygen reduction, with CP1 attaching benzyl derivatives and XCP4 possessing TPA-carbazole substituents at the meso-position of porphyrin, showing similar but more positive ORR potential as compared to the other analogues. Importantly, XCP4 achieved the greatest response current and the largest electron transfer numbers and H 2 O 2 yields among the investigated molecules. Detailed electrochemical measurements suggested that the dipole-induced partial charges on the porphyrin in tandem with the more exposed molecular orbitals on TPA contributed to this enhancement, with the former attracting more protons to the affinity of reactive sites and the latter increasing the collision frequency between the electrocatalyst and H + in solution. This is the first attempt to integrate the intermolecular forces with more exposed molecular orbitals in altering the electrochemical process.

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“…Reviewing and comparing the previous researches on hydrocarbon oxidation, although there were a lot of the influencing factors on the performances of catalysts and the interactions of the factors were complex 49 , it is worthy to use RSM optimizing the reaction conditions of ethyl benzene oxidation catalyzed by Mn TPFPP/mCS catalyst, including the our previous research works 34 , 35 , 53 , 54 , and maybe even some of other research works 1 – 25 . Because the method could tune the external factors (oxidation reaction conditions) to the optimal degree, probably letting the catalysts to make full use of the optimal external reaction conditions 55 .…”

Section: Resultsmentioning

confidence: 99%

Full use of factors promoting catalytic performance of chitosan supported manganese porphyrin

Huang

Wang

et al. 2020

Sci Rep

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in order to make full use of the impact of internal and external factors on the performance of title catalyst for ethyl benzene oxidation, the key internal influencing factors on the catalytic performance were modulated by coordinating and grafting manganese porphyrin to mesoporous and macroporous chitosan, and the important external factors (i.e. oxidation reaction conditions) were optimized using Response Surface Methodology. Under the Response Surface Methodology optimized oxidation reaction conditions (176.56 °C, 0.59 MPa, and 0.25 mg amount of manganese porphyrin), the catalyst could be used at least five times. The ethyl benzene conversion, catalyst turnover numbers, and yields reached up to 51.2%, 4.37 × 10 6 and 36.4% in average, respectively. Compared with the other optimized oxidation reaction conditions, the corresponding values increased 17%, 26% and 53%. Relative to the manganese porphyrin, the catalytic performance and efficiency of the immobilized catalyst had notably increased. High-efficiency and high-selectivity oxidation of ethyl benzene (EB) has been still paid a great attention 1-6. There were so many advanced catalysts and catalytic ethyl benzene oxidation technologies 1-25 , some of which could even offer high yields of products 1-6. However, up to date the oxidation techniques used are not very satisfactory yet: There were mainly lack of cleaner production techniques, for examples, O 2 was not used as oxidant, toxic solvents were used, some energy saving and emission reduction had not been done, and so on. Therefore, the catalyst preparation 21-25 , the catalytic oxidation system and the oxidation conditions 7-20 , which are satisfactorily meeting to the cleaner production process should be comprehensively considered. Based on the above considerations, the internal influencing factors on the catalytic performance of catalyst should be further reasonably tuned, and the external influencing factors should be optimized via Response Surface Methodology (RSM). Because RSM has been successfully used in other catalysis fields: It has been used for optimization of the various reaction conditions and prediction of interactions between the influencing reaction condition parameters based on constructing a suitable model, evaluating the effects of key factors and searching the optimum reaction conditions. The better catalysis responses have achieved 26-29. These considerations and the various optimizations above will probably bring the advanced catalysis techniques 7-25 forwards better catalytic results and excellent various applications in practical chemistry industry. Due to a great deal of attention to the environmental issues, for modern companies which are manufacturing the products of acetophenone and phenylethanol via ethyl benzene oxidation, a set of strict modern technique of cleaner production has to be requested. Under the preconditions, the immobilized metalloporphyrins and their catalysis systems, which are usually not added any additives, co-reductants, and solvents, but oxygen molecules...

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Study on maximizing catalytic performance of cobalt(II) 5,10,15,20-tetrakis(4-pyridyl)porphyrin for cyclohexane oxidation

Cited by 24 publications

References 44 publications

Promotion of Catalytic Oxygen Reduction Reactions: The Utility of Proton Management Substituents on Cobalt Porphyrins

Promotion of Catalytic Oxygen Reduction Reactions: The Utility of Proton Management Substituents on Cobalt Porphyrins

Enhanced Oxygen Reduction Reaction Performance Using Intermolecular Forces Coupled with More Exposed Molecular Orbitals of Triphenylamine in Co-porphyrin Electrocatalysts

Full use of factors promoting catalytic performance of chitosan supported manganese porphyrin

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