Remarkably improved photocatalytic selective oxidation of toluene to benzaldehyde with O2over metal-free delaminated g-C3N4nanosheets: synergistic effect of enhanced textural properties and charge carrier separation

Ghalta, Rajat; Srivastava, Rajendra

doi:10.1039/d2cy01801b

“…44 N 1s was deconvoluted into three peaks, 400.8 eV (NH x , amine functional groups), 399.8 (NC 3 , tertiary nitrogen), and 398.5 eV (pyridinic N). 45 The dominance of the pyridinic N is in accordance with the urea-derived pristine CN. The high-resolution spectrum for C 1s is composed of three peaks.…”

Section: Resultsmentioning

confidence: 82%

“…46 The peak at 284.47 is due to the overlapping of Ru 3d and C 1s and the high intensity is due to the merger of Ru and C signals. 45 Furthermore, the greater peak intensity of C 1s in 3% Ru@ZnO(1.5)/CN (Fig. S6e †) than that of 1% Ru@ZnO(1.5)/CN conrms this observation.…”

Section: Physicochemical Characterizationmentioning

confidence: 67%

“…The decay curves were fitted using a mathematical equation that accounts for the contribution of discrete emissive species. 45 The pre-exponential factors and the time of excited-state luminescence decay were determined for each component. The average decay time, 〈 τ 〉, was calculated using , and the fractional contribution for each decay was obtained using .…”

Section: Resultsmentioning

confidence: 99%

“…The relationship between carrier concentration (N) and electrical conductivity (s) can be expressed using the equation s = Nem, where "e" is the charge and m denotes carrier mobility. 45 Therefore, in 3% Ru@ZnO(1.5)/CN, a signicantly higher charge carrier generation and migration was observed during the light illumination. In conclusion, Ru NPs promoted the mobility of the produced charge carriers and improved the catalyst's performance.…”

Section: Photoelectrochemical Characterizationmentioning

confidence: 89%

“…A that accounts for the contribution of discrete emissive species. 45 The pre-exponential factors and the time of excited-state luminescence decay were determined for each component. The average decay time, hsi, was calculated using hsi ¼…”

Section: Optical Characterizationmentioning

confidence: 99%

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Triazine Frameworks for the Photocatalytic Selective Oxidation of Toluene

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Investigations into the selective oxidation of inert sp3 C–H bonds using polymer photocatalysts under mild conditions have been limited. Additionally, the structure–activity relationship of photocatalysts often remains insufficiently explored. Here, a series of thiophene‐based covalent triazine frameworks (CTFs) are used for the efficient and selective oxidation of hydrocarbons to aldehydes or ketones under ambient aerobic conditions. Spectroscopic methods conducted in situ and density functional theory (DFT) calculations revealed that the sulfur atoms within the thiophene units play a pivotal role as oxidation sites due to the generation of photogenerated holes. The effect of photogenerated holes on photocatalytic toluene oxidation was investigated by varying the length of the spacer in a CTF donor–acceptor based photocatalyst. Furthermore, the manipulation of reactive oxygen species was employed to enhance selectivity by weakening the peroxidative capacity. As an illustrative example, this study successfully demonstrated the synthesis of a precursor of the neurological drug AMG‐579 using a photocatalytic protocol.

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Triazine Frameworks for the Photocatalytic Selective Oxidation of Toluene

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Huber,

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et al. 2024

Angew Chem Int Ed

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View full text Add to dashboard Cite

Investigations into the selective oxidation of inert sp3 C–H bonds using polymer photocatalysts under mild conditions have been limited. Additionally, the structure–activity relationship of photocatalysts often remains insufficiently explored. Here, a series of thiophene‐based covalent triazine frameworks (CTFs) are used for the efficient and selective oxidation of hydrocarbons to aldehydes or ketones under ambient aerobic conditions. Spectroscopic methods conducted in situ and density functional theory (DFT) calculations revealed that the sulfur atoms within the thiophene units play a pivotal role as oxidation sites due to the generation of photogenerated holes. The effect of photogenerated holes on photocatalytic toluene oxidation was investigated by varying the length of the spacer in a CTF donor–acceptor based photocatalyst. Furthermore, the manipulation of reactive oxygen species was employed to enhance selectivity by weakening the peroxidative capacity. As an illustrative example, this study successfully demonstrated the synthesis of a precursor of the neurological drug AMG‐579 using a photocatalytic protocol.

show abstract

Remarkably improved photocatalytic selective oxidation of toluene to benzaldehyde with O₂over metal-free delaminated g-C₃N₄nanosheets: synergistic effect of enhanced textural properties and charge carrier separation

Abstract: The sustainable production of benzaldehyde by the oxidation of toluene with O2 is a challenging and exciting research area due to the low toluene conversion over the reported catalysts and...

Cited by 26 publications

References 90 publications

Thermocatalytic and photocatalytic chemoselective reduction of cinnamaldehyde to cinnamyl alcohol and hydrocinnamaldehyde over Ru@ZnO/CN

Thermocatalytic and photocatalytic chemoselective reduction of cinnamaldehyde to cinnamyl alcohol and hydrocinnamaldehyde over Ru@ZnO/CN

Triazine Frameworks for the Photocatalytic Selective Oxidation of Toluene

Triazine Frameworks for the Photocatalytic Selective Oxidation of Toluene

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