Semiconducting Polymers for Oxygen Evolution Reaction under Light Illumination

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(3), P. 4204 - 4256

Published: Jan. 13, 2022

Sunlight-driven water splitting to produce hydrogen fuel has stimulated intensive scientific interest, as this technology the potential revolutionize fossil fuel-based energy systems in modern society. The oxygen evolution reaction (OER) determines performance of overall owing its sluggish kinetics with multielectron transfer processing. Polymeric photocatalysts have recently been developed for OER, and substantial progress realized emerging research field. In Review, focus is on photocatalytic technologies materials polymeric OER. Two practical systems, namely, particle suspension film-based photoelectrochemical form two main sections. concept reviewed terms thermodynamics kinetics, are discussed based three key characteristics, light absorption, charge separation transfer, surface oxidation reactions. A satisfactory OER by will eventually offer a platform achieve other advanced applications cost-effective, sustainable, renewable manner using solar energy.

Language: Английский

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Unraveling fundamental active units in carbon nitride for photocatalytic oxidation reactions

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Jan. 12, 2021

Covalently bonded carbon nitride (CN) has stimulated extensive attention as a metal-free semiconductor. However, because of the complexity polymeric structures, acquisition critical roles each molecular constituent in CN for photocatalysis remains elusive. Herein, we clarify fundamental active units by synthesizing with more detailed structures. Enabled microwave synthesis, as-prepared consists distinguishable melem (M1) and its incomplete condensed form (M2). We disclose rather than traditional opinion being involved whole photocatalytic processes, M1 M2 make primary contributions light absorption charge separation, respectively. Meanwhile, oxygen molecules are unusually observed to be activated participating photoexcited processes via electronic coupling mainly M2. As result, such higher activity, which was up 8 times that bulk oxidation tetracycline water.

Language: Английский

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Atomically thin ZnS nanosheets: Facile synthesis and superior piezocatalytic H2 production from pure H2O

Applied Catalysis B Environment and Energy, Journal Year: 2020, Volume and Issue: 277, P. 119250 - 119250

Published: June 16, 2020

Language: Английский

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Point‐Defect Engineering: Leveraging Imperfections in Graphitic Carbon Nitride (g‐C₃N₄) Photocatalysts toward Artificial Photosynthesis

Small, Journal Year: 2021, Volume and Issue: 17(48)

Published: April 28, 2021

Abstract Graphitic carbon nitride (g‐C 3 N 4 ) is a kind of ideal metal‐free photocatalysts for artificial photosynthesis. At present, pristine g‐C suffers from small specific surface area, poor light absorption at longer wavelengths, low charge migration rate, and high recombination rate photogenerated electron–hole pairs, which significantly limit its performance. Among myriad modification strategies, point‐defect engineering, namely tunable vacancies dopant introduction, capable harnessing the superb structural, textural, optical, electronic properties to acquire an ameliorated photocatalytic activity. In view burgeoning development in this pacey field, timely review on state‐of‐the‐art advancement engineering vital significance advance solar energy conversion. Particularly, insights into intriguing roles point defects, synthesis, characterizations, systematic control as well versatile application defective ‐based nanomaterials toward water splitting, dioxide reduction nitrogen fixation will be presented detail. Lastly, conclude with balanced perspective technical scientific hindrances future prospects. Overall, it envisioned that open new frontier uncover novel functionalities nanostructures catalysis.

Language: Английский

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Fully Condensed Poly (Triazine Imide) Crystals: Extended π‐Conjugation and Structural Defects for Overall Water Splitting

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 61(2)

Published: Nov. 9, 2021

Conventional polymerization for the synthesis of carbon nitride usually generates amorphous heptazine-based melon with an abundance undesired structural defects, which function as charge carrier recombination centers to decrease photocatalytic efficiency. Herein, a fully condensed poly (triazine imide) crystal extended π-conjugation and deficient structure defects was obtained by conducting polycondensation in mild molten salt LiCl/NaCl. The melting point binary LiCl/NaCl system is around 550 °C, substantially restrain depolymerization triazine units extend π-conjugation. optimized polymeric exhibits high apparent quantum efficiency 12 % (λ=365 nm) hydrogen production one-step excitation overall water splitting, owing efficient exciton dissociation subsequent fast transfer carriers.

Language: Английский

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Rational Design of Carbon‐Based 2D Nanostructures for Enhanced Photocatalytic CO₂Reduction: A Dimensionality Perspective

Chemistry - A European Journal, Journal Year: 2020, Volume and Issue: 26(44), P. 9710 - 9748

Published: June 8, 2020

Photocatalytic CO2 reduction is a revolutionary approach to solve imminent energy and environmental issues by replicating the ingenuity of nature. The past decade has witnessed an impetus in rise two-dimensional (2D) structure materials as advanced nanomaterials boost photocatalytic activities. In particular, use 2D carbon-based deemed highly favorable, not only green material choice, but also due their exceptional physicochemical electrical properties. This Review article presents diverse range alterations compositions derived from nanomaterials, mainly graphene graphitic carbon nitride (g-C3 N4 ), which have remarkably ameliorated performance. Herein, rational design photocatalyst systems with consideration aspect dimensionality resultant heterostructures at interface are systematically analyzed elucidate insightful perspective on this pacey subject. Finally, conclusion outlook limitations prospects cutting-edge research field highlighted.

Language: Английский

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Intrareticular charge transfer regulated electrochemiluminescence of donor–acceptor covalent organic frameworks

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Nov. 23, 2021

The control of charge transfer between radical anions and cations is a promising way for decoding the emission mechanism in electrochemiluminescence (ECL) systems. Herein, type donor-acceptor (D-A) covalent organic framework (COF) with triphenylamine triazine units designed as highly efficient ECL emitter tunable intrareticular (IRCT). D-A COF demonstrates 123 folds enhancement intensity compared its benzene-based small contrast. Further, COF's crystallinity- protonation-modulated behaviors confirm dependence on donor acceptor units, which rationalized by density functional theory. Significantly, dual-peaked patterns COFs are achieved through an IRCT mediated competitive oxidation mechanism: coreactant-mediated at lower potential direct higher potential. This work provides new fundamental approach to improve efficiency designing next-generation devices.

Language: Английский

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Graphitic carbon nitride (g–C3N4)–based semiconductor as a beneficial candidate in photocatalysis diversity

International Journal of Hydrogen Energy, Journal Year: 2021, Volume and Issue: 47(8), P. 5142 - 5191

Published: Dec. 23, 2021

Language: Английский

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Improved Charge Separation in Poly(heptazine‐triazine) Imides with Semi‐coherent Interfaces for Photocatalytic Hydrogen Evolution

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(47)

Published: Sept. 30, 2022

The construction of heterojunctions is a promising manner to accelerate the separation and transfer charge carriers at interface. Herein, binary poly(heptazine-triazine) imides (PHI/PTI) with semi-coherent interfaces was fabricated via facile two-step salt-melt synthetic process. built-in electric fields interface endow prompt exciton splitting carrier separation. Hence, optimized PHI/PTI-based copolymer presents high apparent quantum yield (AQY=64 %) for visible-light driven hydrogen production, by aids K2 HPO4 as mediator. This study provides physical insights rational promotion photocatalytic performance from viewpoint interfacial engineering junctions on crystalline carbon nitride based semiconductors.

Language: Английский

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Extended Conjugation Tuning Carbon Nitride for Non‐sacrificial H₂O₂Photosynthesis and Hypoxic Tumor Therapy**

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(43)

Published: Aug. 8, 2022

Abstract Artificial photocatalysis offers a clean approach for producing H 2 O . However, the poor selectivity and activity of production hamper traditional industrial applications emerging photodynamic therapy (PDT)/chemodynamic (CDT). Herein, we report C 5 N photocatalyst with conjugated C=N linkage selective efficient non‐sacrificial in both normoxic hypoxic systems. The strengthened delocalization π‐electrons by linkers downshifted band position, thermodynamically eliminating side evolution reaction kinetically promoting water oxidation. As result, had competitive solar‐to‐chemical conversion efficiency 0.55 % overall exhibited far highest under conditions (698 μM h −1 ). was further applied to PDT/CDT outstanding performance apparent cancer cell death synchronous bioimaging. study sheds light on photosynthesis carbon nitrides health applications.

Language: Английский

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