Computational design of graphitic carbon nitride photocatalysts for water splitting

Hartley, Gareth O.; Martsinovich, Natalia

doi:10.1039/c9fd00147f

Cited by 16 publications

(12 citation statements)

References 53 publications

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“…For example, if the band gap is reduced, then the material can absorb photon in the visible range. This can be achieved by either doping − or manipulating the side chains/functional groups as in the covalent organic frameworks. , It has been also reported that doping of g-C 3 N 4 improves its photocatalytic activity in the water splitting reactions. , However, to the best of our knowledge, there is no systematic study on the effect of extra-framework cations on the band gap of PHI-based materials. In this paper, we employed DFT-based calculations to study the electronic structures of K-PHI and systems, where K + is replaced by H, Au + , Mg 2+ , and Ru 3+ , as well as the applicability of these materials in the photocatalysis of water splitting reactions.…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Water Splitting Reaction Catalyzed by Ion-Exchanged Salts of Potassium Poly(heptazine imide) 2D Materials

et al. 2021

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Potassium poly (heptazine imide) (K-PHI), a crystalline two-dimensional carbon–nitride material, is an active photocatalyst for water splitting. The potassium ions in K-PHI can be exchanged with other ions to change the properties of the material and eventually to design the catalysts. We report here the electronic structures of several ion-exchanged salts of K-PHI (K, H, Au, Ru, and Mg) and their feasibility as water splitting photocatalysts, which were determined by density functional theory (DFT) calculations. The DFT results are complemented by experiments where the performances in the photocatalytic hydrogen evolution reaction (HER) were recorded. We show that due to its narrow band gap, Ru-PHI is not a suitable photocatalyst. The water oxidation potentials are straddled between the band edge potentials of H-PHI, Au-PHI, and Mg-PHI; thus, these are active photocatalysts for both the oxygen and hydrogen evolution reactions, whereas K-PHI is active only for the HER. The experimental data show that these are active HER photocatalysts, in agreement with the DFT results. Furthermore, Mg-PHI has shown remarkable performance in the HER, with a rate of 539 μmol/(h·g) and a quantum efficiency of 7.14% at 410 nm light irradiation, which could be due to activation of the water molecule upon adsorption, as predicted by our DFT calculations.

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Section: Introductionmentioning

confidence: 99%

Photocatalytic Water Splitting Reaction Catalyzed by Ion-Exchanged Salts of Potassium Poly(heptazine imide) 2D Materials

et al. 2021

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“…Theoretical investigations of g -C 3 N 4 stretch over the past 13 years and feature a myriad of different g -C 3 N 4 structures and configurations. From pristine g -C 3 N 4 to its defected or chemically doped counterparts, the contemporary literature features theoretical efforts on g -C 3 N 4 monomers, monolayers, , bilayers, and periodic systems (also see comprehensive reviews − ). These studies demonstrate that through computational modeling systematic predictions of g -C 3 N 4 properties can be attained that are both enlightening and highly applicable to real experimental systems, which can contain considerable variations in structure or may be difficult to access synthetically.…”

Section: Introductionmentioning

confidence: 99%

Toward Quantum Confinement in Graphitic Carbon Nitride-Based Polymeric Monolayers

2021

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Graphitic carbon nitride (g-C3N4) has garnered much attention due to its potential as an efficient metal-free photocatalyst. This study examines the evolution of properties in zero-dimensional quantum dots up to sizable clusters that mimic extended g-C3N4 monolayers. We employ density functional theory to investigate systematically the structural, electronic, and optical properties of the g-C3N4-based melamine and heptazine building blocks using a “bottom-up” construction of polymeric monolayers. The results from our computations indicate that the melamine- and heptazine-based polymeric g-C3N4 systems must be reduced to at least 2.74 and 4.00 nm, respectively, to observe an increase of its optical gap with a size reduction. The present study also examines the nature of the electronic transitions exhibited by g-C3N4-based monolayers through full natural transition orbital and density of state analyses. The most promising sites for water splitting and subsequent chemical doping studies are identified, which generally correspond to the nitrogen and carbon atoms, respectively.

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“…[21][22][23][24][25][26][27][28] Fortunately, the construction of heterojunctions or modications can improve the aforesaid problems. 29 The separation and storage of the generated hydrogen molecules in the photocatalytic water splitting processes are also crucial. In order to avoid the reverse reaction and possible dangerous explosion, hydrogen should be isolated from the oxygen products during water oxidation.…”

Section: Introductionmentioning

confidence: 99%

“…21–28 Fortunately, the construction of heterojunctions or modifications can improve the aforesaid problems. 29…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic hydrogen production and storage in carbon nanotubes: a first-principles study

Song

Fan

et al. 2022

RSC Adv.

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Computational design of graphitic carbon nitride photocatalysts for water splitting

Abstract: A series of structures based on graphitic carbon nitride (g-C3N4), a layered material composed of linked carbon-nitrogen heterocycles arranged in a plane, were investigated by density functional theory calculations. g-C3N4...

Cited by 16 publications

References 53 publications

Photocatalytic Water Splitting Reaction Catalyzed by Ion-Exchanged Salts of Potassium Poly(heptazine imide) 2D Materials

Photocatalytic Water Splitting Reaction Catalyzed by Ion-Exchanged Salts of Potassium Poly(heptazine imide) 2D Materials

Toward Quantum Confinement in Graphitic Carbon Nitride-Based Polymeric Monolayers

Photocatalytic hydrogen production and storage in carbon nanotubes: a first-principles study

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