Supramolecular organization of melem for the synthesis of photoactive porous carbon nitride rods

Xia, Jiawei; Mark, Gabriel; Volokh, Michael; Fang, Yuanxing; Chen, Haiqun; Wang, Xinchen; Shalom, Menny

doi:10.1039/d1nr06974h

Cited by 23 publications

(11 citation statements)

References 47 publications

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“…Melem was synthesized via thermal condensation of melamine under a nitrogen atmosphere at 425 °C for 12 h; the target temperature of 425 °C was reached at a heating rate of 5 °C min À1 . [11] It was characterized by X-ray diffraction (XRD), Fouriertransform infrared spectroscopy (FTIR) (Figure 1a,b), X-ray photoelectron spectroscopy (XPS), and NMR (Figure S1 and S2, Supporting Information). [16][17][18]…”

Section: Melemmentioning

confidence: 99%

“…The sharp vibrational peak observed at 792 cm À1 in all samples is attributed to the heptazine out-of-plane vibrations. [11,21] The peaks in the 1100-1600 cm À1 region are associated with the in-plane vibrations of heterocycles. [22] The peaks in the 1600-1700 cm À1 range are assigned to the NH bending modes, [23] and the broad peaks centered around 2800-3500 cm À1 arise from NH stretching vibration.…”

Section: Precursorsmentioning

confidence: 99%

“…[7][8][9][10] Such a synthesis affords a highly ordered CN in high yields thanks to the increased π-π interactions between the reactant molecules, lowering their propensity to sublimate compared with traditional small molecules. [11][12][13] However, although well-ordered repeating quasi-2D structures are beneficial for charge transfer, [14] they lead to a low S A and hence, few active sites for heterogeneous (photo)catalysis. Efficient CN-based photocatalysts should strike an optimal compromise between their structural order and the concentration of surface defects that are beneficial as active catalytic sites.…”

Section: Introductionmentioning

confidence: 99%

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Halogen–Hydrogen Bonding for the Synthesis of Efficient Polymeric Carbon‐Nitride Photocatalysts

et al. 2022

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Carbon nitride (CN) materials demonstrate great promise as photocatalysts for various reactions. However, synthesizing a CN with high dispersibility in water, large specific surface area, ordered morphology, and high catalytic activity remains a challenge. Melem (2,5,8‐triamino‐tri‐s‐triazine) has emerged as a monomer for the synthesis of CN materials owing to its high thermal stability, which favors controlled condensation over sublimation and decomposition at high temperatures. Herein, the synthesis of porous CN materials is shown with high dispersibility in water and excellent photocatalytic activity for the hydrogen evolution reaction (HER). To this end, various supramolecular assemblies are designed which are composed of melem combined with different hydrohalogenic acids as precursors of CNs. The results show that the HX (HX (aq), where X = Cl, Br, I) type directs the morphology, optical, and electronic properties of the resulting CN materials, particularly their surface area and photophysical properties. Moreover, the presence of HX results in a CN with a larger amount of free NH2 groups, which allow good dispersibility in water and act as linking groups to a photodeposited Pt cocatalyst. The elucidation of the optimum acid concentration and type leads to the synthesis of a CN with high and stable photocatalytic HER activity.

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Section: Melemmentioning

confidence: 99%

Section: Precursorsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Halogen–Hydrogen Bonding for the Synthesis of Efficient Polymeric Carbon‐Nitride Photocatalysts

et al. 2022

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“…While element- and metal-based systems are restricted by means of tunability (one can tune grain size, crystallinity, surface etc. ), polymeric carbon nitride stands out, since it represents a family of materials . Hence, by rational design approach, it is possible to tune many parameters such as conductivity, charge separation, crystallinity, porosity, absorption, dispersibility, and sheet size. − Some of the most popularized photoredox-based applications of semiconductors include water splitting, − organic synthesis, , photovoltaics, , environmental remediation, CO 2 photoreduction, polymer synthesis, − and photoelectrochemical transformations. , …”

Section: Introductionmentioning

confidence: 99%

Photocatalyst-Incorporated Cross-Linked Porous Polymer Networks

Esen

Kumru

2022

Ind. Eng. Chem. Res.

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The utilization of sunlight to conduct chemistry has been on a stark rise in the era of sustainability. A similar trend is observed in polymer science, mainly to initiate polymerization and modify polymer materials, but mostly relying on the utilization of soluble initiator/activator molecules. Semiconductors, on the other hand, grant a platform for "photoredox" induced chemical pathways, so that reductive and oxidative reactions (as well as radical formation) can be tailored according to band positions. Despite their utilization as dispersed or dissolved phases, immobilization of semiconductors on macroscale solid surfaces is attractive to entail scale-up options. In this Review, semiconductors incorporated in cross-linked porous polymer networks will be summarized both from synthesis and application perspectives.

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“…Several strategies have been adopted to improve the efficiency of PCN in photocatalytic water splitting [ 9 , 10 , 11 , 12 , 13 ]. For example, morphology control is used to regulate specific surface area and adjust energy band structure [ 14 , 15 , 16 ]. Cocatalyst loading is adopted to offer active catalytic sites and facilitate the kinetics of WOR [ 17 ].…”

Section: Introductionmentioning

confidence: 99%

Tunable Carrier Transfer of Polymeric Carbon Nitride with Charge-Conducting CoV2O6∙2H2O for Photocatalytic O2 Evolution

et al. 2022

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Photocatalytic water splitting is one of the promising approaches to solving environmental problems and energy crises. However, the sluggish 4e− transfer kinetics in water oxidation half-reaction restricts the 2e− reduction efficiency in photocatalytic water splitting. Herein, cobalt vanadate-decorated polymeric carbon nitride (named CoVO/PCN) was constructed to mediate the carrier kinetic process in a photocatalytic water oxidation reaction (WOR). The photocatalysts were well-characterized by various physicochemical techniques such as XRD, FT-IR, TEM, and XPS. Under UV and visible light irradiation, the O2 evolution rate of optimized 3 wt% CoVO/PCN reached 467 and 200 μmol h−1 g−1, which were about 6.5 and 5.9 times higher than that of PCN, respectively. Electrochemical tests and PL results reveal that the recombination of photogenerated carriers on PCN is effectively suppressed and the kinetics of WOR is significantly enhanced after CoVO introduction. This work highlights key features of the tuning carrier kinetics of PCN using charge-conducting materials, which should be the basis for the further development of photocatalytic O2 reactions.

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Supramolecular organization of melem for the synthesis of photoactive porous carbon nitride rods

Abstract: Well-ordered porous carbon nitride rods are designed from a supramolecular assembly of large melem molecules as the monomer. It exhibits excellent photocatalytic performance in H2 evolution and CO2 reduction with good stability and selectivity.

Cited by 23 publications

References 47 publications

Halogen–Hydrogen Bonding for the Synthesis of Efficient Polymeric Carbon‐Nitride Photocatalysts

Halogen–Hydrogen Bonding for the Synthesis of Efficient Polymeric Carbon‐Nitride Photocatalysts

Photocatalyst-Incorporated Cross-Linked Porous Polymer Networks

Tunable Carrier Transfer of Polymeric Carbon Nitride with Charge-Conducting CoV2O6∙2H2O for Photocatalytic O2 Evolution

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