Polymeric carbon nitride as a platform for photoelectrochemical water‐splitting cells

Volokh, Michael; Shalom, Menny

doi:10.1111/nyas.14963

Cited by 9 publications

(6 citation statements)

References 46 publications

(125 reference statements)

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“…The assessment of the efficiency of separation of electron–hole (e – –h + ) pairs, generated following photoexcitation, within the prepared materials, was conducted through the resultant photocurrents within a conventional photoelectrochemical cell (PEC) designed for water splitting Figure c reveals that DCDBA5 manifests the most notable photocurrent, attaining a value of ca.…”

Section: Resultsmentioning

confidence: 99%

“…Crystalline carbon nitride materials (CNs), such as poly(heptazine imides) (PHI) and poly(triazine imide) (PTI), have emerged as highly active photocatalysts for various reactions, including water splitting, − CO 2 reduction, − hydrogen peroxide synthesis, − and organic transformation reactions. − Their high activity compared to that of traditional CNs ,− is due to better light-harvesting properties, high specific surface area, suppressed recombination under illumination, and better charge mobility. , The synthesis of CNs with high crystallinity is typically achieved using molten salts as the reaction medium . The final composition and structure are usually determined by how the salt ions are stabilized at the high temperatures where the CN formation reaction takes place.…”

Section: Introductionmentioning

confidence: 99%

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Elucidating the Effect of Crystallinity on the Photoactivity in Poly(heptazine imides)

Li,

Barrio,

Fang

et al. 2023

Energy Fuels

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Poly(heptazine imide) (PHI) polymers have been widely studied, owing to their excellent activity as photocatalysts for various reactions. Their photocatalytic activity has been attributed to defects, optical absorption, or synergistic effects with ions in the reaction media. However, the role of the crystal structure of PHI in photocatalytic activity has not been elucidated. Herein, we reveal a direct correlation between the photocatalytic production of hydrogen (H 2 ) and the crystal structure of PHI. We synthesized polymeric carbon nitride materials focusing on different PHI (001)/(002) crystal plane ratios, high specific surface area, and enhanced light response by copolymerizing organic monomers in a KCl/LiBr molten salt medium. Theoretical and experimental results disclose that the charge carrier dynamics and electron mobility govern the photoactivity of PHI. The best photocatalyst, which had the highest abundance of PHI (100) planes, showed state-of-the-art performance for the hydrogen evolution reaction, with apparent quantum efficiencies of 15.6% at 405 nm and 1.32% at 595 nm, and for the production of H 2 O 2 in pure water under visible light (66.7 μmol g −1 h −1 ).

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Elucidating the Effect of Crystallinity on the Photoactivity in Poly(heptazine imides)

Li,

Barrio,

Fang

et al. 2023

Energy Fuels

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“…Very recently, progress in the different deposition techniques developed in the state of the art to create CN layers has been reported in review articles, to which we would like to refer the reader. [8,123,124] Because the solubility of CN is poor in most solvents, owing to strong Van der Waals interactions, the films prepared by conventional methods are inhomogeneous and weakly attached to the employed transparent electrodes. Our group and others observed that the pyrolysis of supramolecular films prepared with C/N-based monomers allows the construction of CN-based films in robust contact with the electrode.…”

Section: Enhanced Charge Transfer In Photoelectric Devicesmentioning

confidence: 99%

Carbon Nitrides from Supramolecular Crystals: From Single Atoms to Heterojunctions and Advanced Photoelectrodes

Barrio,

Li,

Shalom

2023

Chemistry A European J

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Carbon nitride materials (CN) have become within the last 15 years in one of the most studied photocataysts. While CN absorbs visible light, its low porosity and fast electron – hole recombination hinder its photoelectric performance and have motivated the research in the modification of its physical and chemical properties (such as energy band structure, porosity, or chemical composition) by different means. In this perspective we focus on the utilization of supramolecular crystals as CN precursors to tailor its properties. We elaborate on the features needed in a supramolecular crystal to serve as CN precursor, we delve on the influence of metal‐free crystals in the morphology and porosity of the resulting materials and then discuss the formation of single atoms and heterojunctions when employing a metal‐organic crystal. We finally discuss the performance of CN photoanodes derived from crystals and highlight the current standing challenges in the field.

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“…The stability of PCN on electrodes also needs to be improved. [141] None of the reported energy-storing devices for photocathodic protection can shift the OCP of steel down < −0.8 V versus Ag/AgCl in the dark, but different examples of heterojunctions with TiO 2 can meet that requirement under illumination. [100,104,112,118,122,124,125,127,135] For these materials, charge accumulation might still be relevant to prolong the lifetime of steel, where corrosion could be reasonably prevented during the day and sufficiently slowed down at night.…”

Section: Photocathodic Protection For Anti-corrosionmentioning

confidence: 99%

Photochargeable Semiconductors: in “Dark Photocatalysis” and Beyond

Rogolino

Savateev

2023

Adv Funct Materials

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Photochargeable semiconductors enable energy harvesting and storage in a single material. Charges separated upon absorption of photons can accumulate in highly energetic trap states if morphology, size, and chemical composition are appropriately chosen. For example, electrons can survive for several hours if hole scavengers are used to prevent their recombination with photogenerated holes, and their negative charge is balanced by positive counter‐ions. The first database of charge‐storing semiconductors is recently released, containing information from more than 50 publications within the past 40 years. Now, the database has been updated with more than 90 entries from the latest works on the topic. These materials have been largely utilized in the context of “dark photocatalysis”, that is, redox reactions enabled by photocharged semiconductors long after cessation of light irradiation. Nevertheless, a variety of further potential applications have not received enough visibility, including memory storage, steel anti‐corrosion, sensors, and micromotors. In this review, the key figures of merit of photocharged semiconductors and the empirical relationships found between them is highlighted. After showing the latest advances in dark photocatalysis, it is discussed how other application fields may benefit from these materials. For each area, promising research directions based on the findings from the database are recommended.

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Polymeric carbon nitride as a platform for photoelectrochemical water‐splitting cells

Cited by 9 publications

References 46 publications

Elucidating the Effect of Crystallinity on the Photoactivity in Poly(heptazine imides)

Elucidating the Effect of Crystallinity on the Photoactivity in Poly(heptazine imides)

Carbon Nitrides from Supramolecular Crystals: From Single Atoms to Heterojunctions and Advanced Photoelectrodes

Photochargeable Semiconductors: in “Dark Photocatalysis” and Beyond

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