Regulating Relative Nitrogen Locations of Diazine Functionalized Covalent Organic Frameworks for Overall H₂O₂ Photosynthesis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(41)

Published: Aug. 26, 2023

Nitrogen-heterocycle-based covalent organic frameworks (COFs) are considered promising candidates for the overall photosynthesis of hydrogen peroxide (H2 O2 ). However, effects relative nitrogen locations remain obscured and photocatalytic performances COFs need to be further improved. Herein, a collection functionalized by various diazines including pyridazine, pyrimidine, pyrazine have been judiciously designed synthesized photogeneration H2 without sacrificial agents. Compared with pyrimidine pyrazine, pyridazine embedded in TpDz tends stabilize endoperoxide intermediate species, leading toward more efficient direct 2e- oxygen reduction reaction (ORR) pathway. Benefiting from effective electron-hole separation, low charge transfer resistance, high-efficiency ORR pathway, an excellent production rate 7327 μmol g-1 h-1 solar-to-chemical conversion (SCC) value 0.62 % has achieved TpDz, which ranks one best COF-based photocatalysts. This work might shed fresh light on rational design functional targeting photocatalysts production.

Language: Английский

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Covalent Organic Frameworks Enable Sustainable Solar to Hydrogen Peroxide

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(12)

Published: Dec. 6, 2023

Abstract As a chemical product with rapidly expanding demand in the field of modern energy and environmental applications, hydrogen peroxide (H 2 O ) has garnered widespread attention. However, existing industrial production H is plagued by high consumption, harmful waste emission, severe safety issues, making it difficult to satisfy environmental/economic concept. Artificial photosynthesis offers viable strategy for green sustainable since uses sunlight as an source initiate reaction oxygen water produce . Among various photocatalysts, covalent organic frameworks (COFs), featuring highly ordered skeletons well‐defined active sites, have emerged promising photocatalysts production. This review presents nascent burgeoning area photocatalytic based on COFs. First, brief overview technology provided, followed detailed introduction principles evaluation generation. Subsequently, latest research progress judicious design COFs expounded, particular emphasis manipulating electronic structures redox sites. Finally, outlook challenges future opportunities proposed, hope stimulating further explorations novel molecular‐designed photosynthesis.

Language: Английский

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Engineering 2D Photocatalysts for Solar Hydrogen Peroxide Production

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(23)

Published: April 3, 2024

Abstract Solar energy can be utilized in photocatalysis technology to realize light‐driven hydrogen peroxide (H 2 O ) production, a green chemical synthesis route. Designing high‐performance photocatalysts is critical achieving practical solar H production. During the past decade, significant research progress made photocatalytic materials for Particularly 2D materials‐based stand out due their unique physical and properties. This review highlights intricate relationship between material innovation photochemical It starts with fundamental principles of generation, focusing on crucial steps such as photon absorption, carrier dynamics, surface reactions, challenges that solve at each step. Then, various production are introduced detail. Engineering strategies optimize performance discussed afterward. Finally, future opportunities designing outlined. expected inspire engineering conversion other chemicals.

Language: Английский

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Keto-enamine-based covalent organic framework with controllable anthraquinone moieties for superior H2O2 photosynthesis from O2 and water

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 466, P. 143085 - 143085

Published: April 23, 2023

Language: Английский

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Rejoint of Carbon Nitride Fragments into Multi‐Interfacial Order‐Disorder Homojunction for Robust Photo‐Driven Generation of H₂O₂

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(9)

Published: Nov. 8, 2023

Abstract Photocatalytic technology based on carbon nitride (C 3 N 4 ) offers a sustainable and clean approach for hydrogen peroxide (H 2 O production, but the yield is severely limited by sluggish hot carriers due to weak internal electric field. In this study, novel devised fragmenting bulk C into smaller pieces (CN‐NH then subjecting it directed healing process create multiple order‐disorder interfaces ‐NaK). The resulting junctions in CN‐NH ‐NaK significantly boost charge dynamics facilitate more spatially orderly separated redox centers. As result, demonstrates outstanding photosynthesis of H via both two‐step single‐electron one‐step double‐electron oxygen reduction pathways, achieving remarkable 16675 µmol h –1 g , excellent selectivity (> 91%), prominent solar‐to‐chemical conversion efficiency exceeding 2.3%. These results surpass pristine 158 times outperform previously reported ‐based photocatalysts. This work represents significant advancement catalyst design modification technology, inspiring development efficient metal‐free photocatalysts synthesis highly valued fuels.

Language: Английский

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Mesoporous carbon spheres with programmable interiors as efficient nanoreactors for H2O2 electrosynthesis

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 1, 2024

Abstract The nanoreactor holds great promise as it emulates the natural processes of living organisms to facilitate chemical reactions, offering immense potential in catalytic energy conversion owing its unique structural functionality. Here, we propose utilization precisely engineered carbon spheres building blocks, integrating micromechanics and controllable synthesis explore their functionalities two-electron oxygen reduction reactions. After conducting rigorous experiments simulations, present compelling evidence for enhanced mass transfer microenvironment modulation effects offered by these mesoporous hollow spheres, particularly when possessing a suitably sized architecture. Impressively, pivotal achievement lies successful screening potent, selective, durable reaction catalyst direct medical-grade hydrogen peroxide disinfectant. Serving an exemplary demonstration engineering screening, this work highlights various well-designed carbon-based nanoreactors extensive applications.

Language: Английский

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Boosting photo-self-Fenton-like reaction via ferric-ellagate complex for environmental remediation

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 338, P. 126450 - 126450

Published: Jan. 21, 2024

Language: Английский

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Unveiling Favorable Microenvironment on Porous Doped Carbon Nanosheets for Superior H₂O₂ Electrosynthesis in Neutral Media

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(19)

Published: Feb. 21, 2024

Abstract Designing effective electrocatalysts tailored for targeted reactions requires fundamental insights into the structure dependence of reaction microenvironment. Herein, inspired by finite element simulations, N,O co‐doped carbon nanosheets featuring a hierarchical micro/mesoporous to form an oxygen‐rich and local alkaline‐like microenvironment two‐electron oxygen reduction (2e − ORR) in neutral medium are designed. The situ ex test results confirmed that architecture can elevate pH accelerate generation intermediates (*O 2 , *OOH), leading high‐efficiency H O production. Utilizing this favorable microenvironment, N,O‐CNS 0.5 demonstrated exceptional electrosynthesis performance media, achieving superior yield rate (6705 mmol g catalyst −1 h flow cell). Additionally, comparative experiments density‐functional theory calculations provided confirmation bi‐doping N as active origin responsible electrochemical 2e ORR. This study synergistically manipulates sites, providing opportunity efficient electro‐production medium.

Language: Английский

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Covalent Organic Frameworks for Photocatalytic Hydrogen Peroxide Generation

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(5), P. 2007 - 2049

Published: April 17, 2024

Hydrogen peroxide (H2O2), a valuable chemical, is widely used as powerful oxidizing agent in chemical synthesis, pharmaceuticals, medical disinfection, and environmental treatment industries. Currently, over 95% of H2O2 produced industrially using the anthraquinone process, which associated with its high energy consumption hazardous byproducts. Therefore, photochemical synthesis from water oxygen covalent organic framework based photocatalysts have attracted considerable attention. This review aims to outline recent achievements, challenges future prospects COFs heterogeneous for sustainable generation. We summarize chronological development COFs, different mechanisms involved, detailed experiments quantification methods photocatalytic The puts forward an outlook, highlighting advantages limitations anticipate that this will provide insight into current progress inspire next-generation production.

Language: Английский

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H₂O₂ Photosynthesis from H₂O and O₂ under Weak Light by Carbon Nitrides with the Piezoelectric Effect

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(30), P. 21147 - 21159

Published: July 16, 2024

Driven by the essential need of a green, safe, and low-cost approach to producing H

Language: Английский

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