Low-Temperature Synthesis of Solution Processable Carbon Nitride Polymers

Li, Junyi; Karjule, Neeta; Qin, Jiani; Wang, Ying; Barrio, Jesús; Shalom, Menny

doi:10.3390/molecules26061646

Cited by 13 publications

(10 citation statements)

References 41 publications

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“…In order to study this synthetic approach with a wider variety of precursors, thereby showing its applicability to the synthesis of different materials, we replaced melamine with other precursors commonly employed in the preparation of photoactive polymers, namely urea, [48] dicyandiamide (DCD), [49] acetoguanamine (AGA), [50,51] and 2,4,6‐triaminopyrimidine (TAP), [52,53] and we studied the supramolecular self‐assembly behaviour of the resulting mixture. Amongst those monomers, we observed that only TAP was able to form a bulk hydrogel with cyanobenzoic acid, probably owing to the very similar structure and hydrogen‐bonding ability of TAP and MA [46,54] .…”

Section: Resultsmentioning

confidence: 99%

Efficient Water Cleaning by Self‐standing Carbon Nitride Films Derived from Supramolecular Hydrogels

Dor

Barrio

et al. 2022

Chemistry A European J

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The design of efficient self-standing hybrid systems for water purification that combines good adsorption properties with high photodegradation ability is highly challenging owing to the difficulty in simultaneously controlling the band structure and porosity of a semiconductor while maintaining its self-standing nature. Here, we report the synthesis of carbon-rich carbon nitride self-standing filters from supramolecular hydrogels composed of melamine and cyanobenzoic acid. The influence of the chemical structure on the properties of the hydrogels and the final films was studied by tuning parameters such as monomer nature, molar ratio, and pyrolysis temperature. Thanks to their ability to combine the adsorption and photodegradation of organic pollutants, the prepared self-standing films showed remarkable activity and stability in flow conditions (> 95 % efficiency after 10 consecutive cycles). Additionally, the photocatalytic activity of the films was assessed in the powder form for the hydrogen evolution reaction and photocurrent generation in a photoelectrochemical cell. The reported work opens opportunities for the controlled synthesis of multifunctional filters for water purification and other energy-related and sustainable technologies.

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Section: Resultsmentioning

confidence: 99%

Efficient Water Cleaning by Self‐standing Carbon Nitride Films Derived from Supramolecular Hydrogels

Dor

Barrio

et al. 2022

Chemistry A European J

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“…The C 1s narrow spectrum in Figure 6(a) was deconvoluted into three components: the typical peak at 284.5 eV is assigned to C−C bonded atoms present in adventitious carbon, whereas the peaks 285.8 and 287.5 eV are attributed to C−N=C and C−(N) 3 groups of g‐C 3 N 4 support [36] . The N 1s photoelectron spectrum can be deconvoluted into two peaks centered at approximately 398.5 and 400.2 eV, which related to C−N=C and N−(C) 3 species, indicating the characteristics of graphitic structure of g‐C 3 N 4 [37,38] . Figure 6(c) illustrates the Ni 2p photoelectron spectrum which describes the chemical states of nickel present on the outermost surface of the sample.…”

Section: Resultsmentioning

confidence: 99%

“…[36] The N 1s photoelectron spectrum can be deconvoluted into two peaks centered at approximately 398.5 and 400.2 eV, which related to CÀ N=C and NÀ (C) 3 species, indicating the characteristics of graphitic structure of g-C 3 N 4 . [37,38]…”

Section: Xps Surface Analysismentioning

confidence: 99%

Carbon Monoxide Desorption and Reduction Studies of Graphitic Carbon Nitride Supported Nickel Catalysts for CO Methanation

et al. 2022

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Graphitic carbon nitride (g-C 3 N 4 ) has attracted much attention due to its unique polymeric structure of carbon and nitrogen in the form of heptazine units. In this study, a nickel catalyst supported on graphitic carbon nitride was prepared by a facile impregnation method. Ni/g-C 3 N 4 desorption and reduction behaviors with carbon monoxide (CO) were investigated by temperature-programmed desorption (TPD) and reduction (TPR). The chemisorption study of reduction and desorption behaviors of CO molecules on Ni/g-C 3 N 4 catalyst is essential for CO methanation reaction. The as-prepared Ni/g-C 3 N 4 catalyst was also characterized by X-ray diffraction (XRD), N 2 physisorption, and X-ray photoelectron spectroscopy (XPS). It was found that the utilization of g-C 3 N 4 as a catalyst support enhances the complete reduction of Ni species and CO desorption. This can be attributed to the role of g-C 3 N 4 support as a reducing agent for Ni, as well as its basicity owing to the richness of nitrogen functional group. The good performance of Ni/g-C 3 N 4 catalyst towards CO methanation can be ascribed to the improvement in adsorption and activation of CO molecules on the active sites and the number of surface basic sites.

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“…This difference indicates a modification of the melaminium chloride hemihydrate structure caused by the additional AGA, whose methyl groups disrupt the crystal growth in a three dimensional fashion (Scheme S1, Figure S2, Supporting Infor mation). [25,26] Unfortunately, we could not grow single crystals of melamine:AGA suitable for SCXRD analysis.…”

Section: Resultsmentioning

confidence: 99%

Fluorescent Carbon Nitride Macrostructures Derived from Triazine‐Based Cocrystals

Barrio

Barzilai²,

Karjule

et al. 2021

Advanced Optical Materials

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Graphitic carbon nitrides (CNs) have attracted widespread attention during the last decade, thanks to their potential to address current materials science chal lenges, such as the production of solar fuels by photoelectrochemical means or the catalytic removal of organic pollu tants from water. [1][2][3][4][5] The possibility of tai loring parameters such as charge transfer kinetics, porosity, or energy band positions through approaches including doping, [6] templating, [7] covalent functionalization, [8,9] or the formation of heterojunctions [10] has opened the gate toward the application of CNbased materials in various fields, including bioimaging and electrochemi luminescent devices. [11][12][13][14] However, the rational design of CN materials for these applications remains in its infancy. Typically, to obtain CNbased highly emissive materials, topdown strategies or hydrothermal means are used [15,16] but they do not allow their scalability for industrial applications. Consequently, compatible synthesis with largescale production of CN powders suitable for solidstate fluorescentsensing platforms remains a challenge.During the last few years, our group and others have shown that the utilization of selfassembled supramolecular struc tures for the hightemperature synthesis of CN allows for the preservation of chemical bonds, morphologies, and electronic structures, which permits controlling of CN properties at the molecular level and their largescale production. [17] Notably, highly ordered supramolecular single crystals have been shown to be particularly useful in this regard. [18][19][20] In this work, we exploited these findings to synthesize new triazine based cocrystals composed of melamine and acetoguanamine (AGA), which were subsequently used as precursors for CN via hightemperature reaction. We tuned the precursor crystalline structures to endow the final CNs with a good photolumines cent behavior in both liquid and solid states, as demonstrated by their performance in detecting metal ions (in an aqueous environment) and labeling latent fingerprints (as a solidstate sensing platform). Results and DiscussionMelaminebased cocrystals were prepared by dissolving mela mine with different amounts of AGA in an aqueous solution Carbon nitride (CN) based materials have emerged as efficient photo-and electrocatalysts for various reactions. However, despite their intriguing optical properties (i.e., fluorescence), their utilization as solid-state sensing platforms remains in its infancy, owing to the formation of defect states during the materials synthesis, leading to low emission for the CN powder. Here, a bottom-up synthesis of CN macrostructures with good photoluminescence properties in both liquid and solid state is introduced, from designed triazinebased cocrystals with ordered morphology and tailored chemical composition. Upon calcination at 500 °C, the starting morphology and chemical composition are retained, resulting in the alteration of the HOMO-LUMO distribution of the CN materials, as further supporte...

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Low-Temperature Synthesis of Solution Processable Carbon Nitride Polymers

Cited by 13 publications

References 41 publications

Efficient Water Cleaning by Self‐standing Carbon Nitride Films Derived from Supramolecular Hydrogels

Efficient Water Cleaning by Self‐standing Carbon Nitride Films Derived from Supramolecular Hydrogels

Carbon Monoxide Desorption and Reduction Studies of Graphitic Carbon Nitride Supported Nickel Catalysts for CO Methanation

Fluorescent Carbon Nitride Macrostructures Derived from Triazine‐Based Cocrystals

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