Synthesis of Cu Single Atoms Supported on Mesoporous Graphitic Carbon Nitride and Their Application in Liquid-Phase Aerobic Oxidation of Cyclohexene

Büker, Julia; Huang, Xiubing; Bitzer, Johannes; Kleist, Wolfgang; Mühler, Martin; Peng, Baoxiang

doi:10.1021/acscatal.1c01468

Cited by 83 publications

(49 citation statements)

References 60 publications

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“…Cu 2p XPS spectra are quite different before and after use of Cu@Cu 2 O/C-24 as the antibacterial sample. The Cu 2p 3/2 can be fitted into two peaks at binding energies of 932.5 and 935.0 eV corresponding to Cu + /Cu 0 and Cu 2+ species. − In general, Cu 2p 3/2 XPS cannot differentiate between Cu + and Cu 0 due to the overlapping binding energies and similar splitting of 20 eV . Therefore, Auger Cu LMM spectra were used to confirm the presence of Cu + and Cu 0 .…”

Section: Results and Discussionmentioning

confidence: 99%

“…41−43 In general, Cu 2p 3/2 XPS cannot differentiate between Cu + and Cu 0 due to the overlapping binding energies and similar splitting of 20 eV. 44 Therefore, Auger Cu LMM spectra were used to confirm the presence of Cu + and Cu 0 . As shown in Figure 4B, the binding energies at 570 and 568.1 eV were attributed to Cu + and Cu 0 , respectively.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

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Anchoring Core–Shell Cu@Cu₂O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Sun

Jia

Zhang

et al. 2021

ACS Appl. Nano Mater.

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The unique physicochemical properties and relatively higher biosafety endow carbon-based nanomaterials with much worldwide attention. However, studies of the synthesis and functionalization of carbon nanosheets are still very limited, which largely impedes the development of carbon-based materials for antibacterial applications. In this work, carbon nanosheets decorated with core−shell Cu@Cu 2 O nanoparticles (Cu@Cu 2 O/ C) were prepared by a facial hydrothermal method using copper Dgluconate. The in situ-generated carbon nanosheets feature a homogeneous size distribution with an average diameter of 3 μm and thickness of 5 nm. The particle size of Cu@Cu 2 O is mainly distributed between 10.5 and 13.5 nm. Particularly, these nanosheets could not only effectively anchor Cu@Cu 2 O core− shell structured nanoparticles but also bring more edge active sites, which could promote the generation of free radicals. The asprepared Cu@Cu 2 O/C verified by varieties of characterizations were used as antibacterial samples to kill the Gram-negative bacterium Escherichia coli and the Gram-positive bacterium S. aureus with antibacterial efficiencies of up to 100 and 96.0%, respectively, within 12 min in the dark condition. A possible antibacterial mechanism of the • OH-dominated radical combined with the sharp edges of carbon nanosheets was confirmed by a series of control experiments. Overall, the present work provides a simple strategy to prepare carbon-based antibacterial agents, which sheds light on the understanding of the antibacterial mechanism of carbon-based nanomaterials.

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Section: Results and Discussionmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 99%

Anchoring Core–Shell Cu@Cu₂O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Sun

Jia

Zhang

et al. 2021

ACS Appl. Nano Mater.

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“…Prior to the in situ measurement, ATR-IR spectra of reference samples in acetonitrile were recorded (Figure S21) to assign the characteristic bands to the reactant and the oxidation products, which are summarized in Table S3. [51] The identification of reaction products and especially of the cyclohex-2-ene-1-hydroperoxide intermediate was discussed recently. [51] The reaction progress of cyclohexene oxidation was continuously monitored by recording IR spectra every 2 min.…”

Section: Time-resolved In Situ Atr-ir Spectroscopymentioning

confidence: 99%

“…[51] The identification of reaction products and especially of the cyclohex-2-ene-1-hydroperoxide intermediate was discussed recently. [51] The reaction progress of cyclohexene oxidation was continuously monitored by recording IR spectra every 2 min. Figure 10 shows the first-derivative spectra after admitting a solution of cyclohexene in acetonitrile containing Sr40 nanoparticles as the catalyst (Figure S22).…”

Section: Time-resolved In Situ Atr-ir Spectroscopymentioning

confidence: 99%

Liquid‐Phase Cyclohexene Oxidation with O₂ over Spray‐Flame‐Synthesized La_1−xSr_xCoO₃ Perovskite Nanoparticles

Büker

Alkan

Chabbra

et al. 2021

Chemistry A European J

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La1−xSrxCoO3 (x=0, 0.1, 0.2, 0.3, 0.4) nanoparticles were prepared by spray‐flame synthesis and applied in the liquid‐phase oxidation of cyclohexene with molecular O2 as oxidant under mild conditions. The catalysts were systematically characterized by state‐of‐the‐art techniques. With increasing Sr content, the concentration of surface oxygen vacancy defects increases, which is beneficial for cyclohexene oxidation, but the surface concentration of less active Co2+ was also increased. However, Co2+ cations have a superior activity towards peroxide decomposition, which also plays an important role in cyclohexene oxidation. A Sr doping of 20 at. % was found to be the optimum in terms of activity and product selectivity. The catalyst also showed excellent reusability over three catalytic runs; this can be attributed to its highly stable particle size and morphology. Kinetic investigations revealed first‐order reaction kinetics for temperatures between 60 and 100 °C and an apparent activation energy of 68 kJ mol−1 for cyclohexene oxidation. Moreover, the reaction was not affected by the applied O2 pressure in the range from 10 to 20 bar. In situ attenuated total reflection infrared spectroscopy was used to monitor the conversion of cyclohexene and the formation of reaction products including the key intermediate cyclohex‐2‐ene‐1‐hydroperoxide; spin trap electron paramagnetic resonance spectroscopy provided strong evidence for a radical reaction pathway by identifying the cyclohexenyl alkoxyl radical.

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“…To identify a superoxide intermediate, in situ IR spectroscopy has been used in combination with isotope labeling using 18 O 2 over a SrMnO 3 catalyst [95k] . By applying in situ ATR‐IR spectroscopy, the reaction progress in cyclohexene oxidation was monitored [114] . Vibrational spectroscopy furthermore enabled the study of the interplay of a Co‐based catalyst with DMF as the solvent [107g] .…”

Section: Thermal Catalysismentioning

confidence: 99%

A Perspective on Heterogeneous Catalysts for the Selective Oxidation of Alcohols

Najafishirtari

Ortega

Douthwaite

et al. 2021

Chemistry A European J

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Selective oxidation of higher alcohols using heterogeneous catalysts is an important reaction in the synthesis of fine chemicals with added value. Though the process for primary alcohol oxidation is industrially established, there is still a lack of fundamental understanding considering the complexity of the catalysts and their dynamics under reaction conditions, especially when higher alcohols and liquid-phase reaction media are involved. Additionally, new materials should be developed offering higher activity, selectivity, and stability. This can be achieved by unraveling the structure-performance correlations of these catalysts under reaction conditions. In this regard, researchers are encouraged to develop more advanced characterization techniques to address the complex interplay between the solid surface, the dissolved reactants, and the solvent. In this mini-review, we report some of the most important approaches taken in the field and give a perspective on how to tackle the complex challenges for different approaches in alcohol oxidation while providing insight into the remaining challenges.

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Synthesis of Cu Single Atoms Supported on Mesoporous Graphitic Carbon Nitride and Their Application in Liquid-Phase Aerobic Oxidation of Cyclohexene

Cited by 83 publications

References 60 publications

Anchoring Core–Shell Cu@Cu₂O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Anchoring Core–Shell Cu@Cu₂O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Liquid‐Phase Cyclohexene Oxidation with O₂ over Spray‐Flame‐Synthesized La_1−xSr_xCoO₃ Perovskite Nanoparticles

A Perspective on Heterogeneous Catalysts for the Selective Oxidation of Alcohols

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Synthesis of Cu Single Atoms Supported on Mesoporous Graphitic Carbon Nitride and Their Application in Liquid-Phase Aerobic Oxidation of Cyclohexene

Cited by 83 publications

References 60 publications

Anchoring Core–Shell Cu@Cu2O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Anchoring Core–Shell Cu@Cu2O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Liquid‐Phase Cyclohexene Oxidation with O2 over Spray‐Flame‐Synthesized La1−xSrxCoO3 Perovskite Nanoparticles

A Perspective on Heterogeneous Catalysts for the Selective Oxidation of Alcohols

Contact Info

Product

Resources

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Anchoring Core–Shell Cu@Cu₂O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Anchoring Core–Shell Cu@Cu₂O Nanoparticles to Two-Dimensional Carbon Nanosheets for Bacterial Disinfection

Liquid‐Phase Cyclohexene Oxidation with O₂ over Spray‐Flame‐Synthesized La_1−xSr_xCoO₃ Perovskite Nanoparticles