A true oxygen-linked heptazine based polymer for efficient hydrogen evolution

Battula, Venugopala Rao; Kumar, Sunil; Chauhan, Deepak Kumar; Samanta, Soumadri; Kailasam, Kamalakannan

doi:10.1016/j.apcatb.2018.11.027

Cited by 60 publications

(42 citation statements)

References 63 publications

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“…As reported earlier, OLHP exhibits an intense diffraction peak at 2q ¼ 27.1 , which has been indexed to the (002) stacked plane of conjugated heptazine units as in graphite. 36 Aer decorating S,N-GQDs with different proportions, no shi in the peak at 2q ¼ 27.1 was observed, which signies that there is no effect on the stacking arrangement of heptazine sheets in OLHP. In Fig.…”

Section: Resultsmentioning

confidence: 91%

“…42 OLHP shows absorption peaks which correspond to the functional groups of the tri-s-triazine structure (804 cm À1 ), heptazine heterocycles (1633-1236 cm À1 ), and ternary hydroxyl group (3000-3400 cm À1 ). 36 The OLHP/S,N-GQDs exhibit an FTIR spectrum with characteristics peaks of both OLHP and S,N-GQDs. The presence of C]S stretching in OLHP/S,N-GQDs conrms the decoration of S,N-GQDs on OLHP.…”

Section: Resultsmentioning

confidence: 99%

“…The conduction band minima (CBM) and valence band maxima (VBM) for OLHP lie at À1.32 V (vs. Ag/ AgCl) and 1.35 V (vs. Ag/AgCl), respectively, with an optical band gap of 2.67 eV. 36 The corresponding band positions for both the photosensitizer and photocatalyst (with respect to NHE) are shown in Fig. 5b, which clearly satises the requirement for the possible feasibility of electron transfer through the dye sensitization process as the CBM of S,N-GQDs lies just more negative to the CBM of OLHP.…”

Section: Resultsmentioning

confidence: 99%

“…Firstly, OLHP-550 was prepared using the previously reported method. 36 S, N codoped graphene quantum dots (S,N-GQDs) were synthesized following the reported method by Qu et al 42 Then with asprepared OLHP, a specic volume of S,N-GQDs was added and then sonicated for 1 h. Finally, the suspension was transferred into a teon-lined stainless steel autoclave and kept at 100 C for 6 h in an air oven ( Fig. 1).…”

Section: Materials and Sample Preparationmentioning

confidence: 99%

“…34,35 Following this work, Kailasam and group reported the synthesis of true O-linked heptazine polymer, OLHP (from cyameluric acid as a precursor) as an efficient structural variant of g-CN with enhanced photocatalytic activity for hydrogen evolution. 36 It was argued that the presence of bridging O-atoms in OLHP renders better charge separation and a lifetime to charge carriers to be efficiently utilized in water reduction reaction as compared to g-CN and as a result, OLHP produces 41-fold higher H 2 compared to g-CN. However, like g-CN, OLHP required the presence of Pt-metal as a co-catalyst for water splitting.…”

Section: Introductionmentioning

confidence: 99%

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Quantum dot-sensitized O-linked heptazine polymer photocatalyst for the metal-free visible light hydrogen generation

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Section: Resultsmentioning

confidence: 91%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Materials and Sample Preparationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Quantum dot-sensitized O-linked heptazine polymer photocatalyst for the metal-free visible light hydrogen generation

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The Design of Supramolecular Assemblies with Metal Salt as Precursors Enables The Growth of Stable Polymeric Carbon Nitride Photoanodes

Garg,

Shmila,

Mark

et al. 2023

Advanced Sustainable Systems

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Polymeric carbon nitrides (CN) have gained significant interest as photoanodes in photoelectrochemical cells (PEC). A widely researched approach for synthesizing CN films with controlled optical and photoelectrochemical properties relies on using supramolecular assemblies as the precursors for thermal polymerization over a transparent conductive substrate. However, the formation of supramolecular assemblies is highly dependent on the temperature and solubility in a given solvent, limiting the full potential of this method. Moreover, the intercalation of metal ions is challenging due to the use of polar solvents. Here, this study shows a new way of synthesizing supramolecular assemblies with metal ions using a solvothermal approach. The solvent, monomer composition, salt quantity, reaction temperature, and film thickness are varied in this study. As a result, well‐attached, uniform CN films with good optoelectronic properties are achieved. The synthesized photoactive CN films exhibit very low onset potentials and reach ≈0.13, ≈0.15, and 0.30 ± 0.01 mA cm−2 photocurrents in 0.1 m phosphate buffer (neutral) solution, 0.1 m KOH(aq) (basic) solution, and 0.1 m KOH solution containing 10 vol.% triethanolamine as the hole scavenger, respectively.

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Hydroxyl Radical Mediated Heterogeneous Photocatalytic Baeyer–Villiger Oxidation over Covalent Triazine/Heptazine‐Based Frameworks

Tang,

Jiang,

Gao

et al. 2024

Angewandte Chemie

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The Baeyer‐Villiger oxidation of ketones to the corresponding lactones/esters is a classic and essential reaction in the chemical industry. However, this oxidation process has not yet been achieved in ambient conditions with the aid of oxygen and heterogeneous photocatalysts. In this study, we developed an organic photocatalytic system using covalent triazine/heptazine‐based frameworks (CTF‐TB/CHF‐TB) to enable the B‐V oxidation reaction under mild conditions through a cascade reaction pathway. Experimental data and theoretical calculations showed that heptazine/triazine units can "chelate” and decompose the in situ generated H2O2 into hydroxyl radicals (•OH). Compared to conventional methods that primarily involve metal‐activated benzaldehyde at elevated temperatures (e.g., 60 oC), the •OH generated in our study can readily cleave the C‐H bond of benzaldehyde, forming an active intermediate that drives subsequent sequential processes: O2→H2O2→•OH→Ph‐CO•→Ph‐COOO•. By employing this photocatalytic process, a yield of 91% and a selectivity of over 99 % were obtained in the oxidation of cyclohexanone to caprolactone at room temperature. This performance is comparable to the state‐of‐the‐art catalysts, and our CHF‐TB catalyst demonstrates impressive reusability, maintaining a high yield after 5 consecutive runs. This work presents a straightforward approach for C‐H cleavage by organocatalysts to produce ε‐caprolactone in a mild manner by Baeyer‐Villiger oxidation.

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A true oxygen-linked heptazine based polymer for efficient hydrogen evolution

Cited by 60 publications

References 63 publications

Quantum dot-sensitized O-linked heptazine polymer photocatalyst for the metal-free visible light hydrogen generation

Quantum dot-sensitized O-linked heptazine polymer photocatalyst for the metal-free visible light hydrogen generation

The Design of Supramolecular Assemblies with Metal Salt as Precursors Enables The Growth of Stable Polymeric Carbon Nitride Photoanodes

Hydroxyl Radical Mediated Heterogeneous Photocatalytic Baeyer–Villiger Oxidation over Covalent Triazine/Heptazine‐Based Frameworks

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