Developing Ni single-atom sites in carbon nitride for efficient photocatalytic H2O2 production

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 6, 2023

Photocatalytic two-electron oxygen reduction to produce high-value hydrogen peroxide (H2O2) is gaining popularity as a promising avenue of research. However, structural evolution mechanisms catalytically active sites in the entire photosynthetic H2O2 system remains unclear and seriously hinders development highly-active stable photocatalysts. Herein, we report high-loading Ni single-atom photocatalyst for efficient synthesis pure water, achieving an apparent quantum yield 10.9% at 420 nm solar-to-chemical conversion efficiency 0.82%. Importantly, using situ synchrotron X-ray absorption spectroscopy Raman directly observe that initial Ni-N3 dynamically transform into high-valent O1-Ni-N2 after O2 adsorption further evolve form key *OOH intermediate before finally forming HOO-Ni-N2. Theoretical calculations experiments reveal structure reduces formation energy barrier suppresses O=O bond dissociation, leading improved production activity selectivity.

Язык: Английский

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An organic perspective on photocatalytic production of hydrogen peroxide

Nature Catalysis, Год журнала: 2023, Номер 6(7), С. 553 - 558

Опубликована: Июль 25, 2023

Язык: Английский

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Recent advances, application and prospect in g-C3N4-based S-scheme heterojunction photocatalysts

Separation and Purification Technology, Год журнала: 2023, Номер 330, С. 125302 - 125302

Опубликована: Окт. 12, 2023

Язык: Английский

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Covalent Organic Frameworks Enable Sustainable Solar to Hydrogen Peroxide

Advanced Functional Materials, Год журнала: 2023, Номер 34(12)

Опубликована: Дек. 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.

Язык: Английский

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Ambient Preparation of Benzoxazine‐based Phenolic Resins Enables Long‐term Sustainable Photosynthesis of Hydrogen Peroxide

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(23)

Опубликована: Март 25, 2023

Rational design of polymer structures at the molecular level promotes iteration high-performance photocatalyst for sustainable photocatalytic hydrogen peroxide (H2 O2 ) production from oxygen and water, which also lays basis revealing reaction mechanism. Here we report a benzoxazine-based m-aminophenol-formaldehyde resin (APFac) polymerized ambient conditions, exhibiting superior H2 yield long-term stability to most polymeric photocatalysts. Benzoxazine structure was identified as crucial active segment in APFac. Favorable adsorption oxygen/intermediates on benzoxazine commendable product selectivity accelerated kinetically stepwise single-electron reduction reaction. The proposed phenolic provides possibility batches industrial application, sheds light de novo analysis metal-free

Язык: 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, Год журнала: 2023, Номер 36(9)

Опубликована: Ноя. 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.

Язык: Английский

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Vinyl‐Group‐Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(21)

Опубликована: Март 16, 2024

The artificial photosynthesis of H

Язык: Английский

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Mixed‐Linker Strategy for the Construction of Sulfone‐Containing D–A–A Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Peroxide Production

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(22)

Опубликована: Фев. 28, 2024

Abstract The solar‐driven photocatalytic production of hydrogen peroxide (H 2 O ) from water and oxygen using semiconductor catalysts offers a promising approach for converting solar energy into storable chemical energy. However, the efficiency H is often restricted by low photo‐generated charge separation, slow surface reactions inadequate stability. Here, we developed mixed‐linker strategy to build donor‐acceptor‐acceptor (D–A–A) type covalent organic framework (COF) photocatalyst, FS‐OHOMe‐COF. FS‐OHOMe‐COF structure features extended π–π conjugation that improves mobility, while introduction sulfone units not only as active sites facilitates with but also bolsters stability through increased interlayer forces. resulting has exciton binding energy, long excited‐state lifetime high photo‐stability leads performance (up 1.0 mM h −1 an output 19 after 72 hours irradiation. Furthermore, catalyst demonstrates stability, which sustained activity over 192 experiment.

Язык: Английский

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A Novel Dual-Channel Carbon Nitride Homojunction with Nanofibrous Carbon for Significantly Boosting Photocatalytic Hydrogen Peroxide Production

Advanced Fiber Materials, Год журнала: 2024, Номер 6(2), С. 387 - 400

Опубликована: Янв. 9, 2024

Язык: Английский

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Interface Chemical Bond Enhanced Ions Intercalated Carbon Nitride/CdSe‐Diethylenetriamine S‐Scheme Heterojunction for Photocatalytic H₂O₂ Synthesis in Pure Water

Advanced Functional Materials, Год журнала: 2024, Номер 34(24)

Опубликована: Фев. 19, 2024

Abstract Photosynthesis of hydrogen peroxide (H 2 O ) is regarded as an economically efficient and environmentally friendly synthesis method. However, the scalability photocatalytic H production (PHP) hindered by sluggish reaction kinetics rapid recombination photogenerated charge carriers. In this study, organic amine‐constrained ions intercalated carbon nitride/CdSe‐diethylenetriamine (K + /I − ‐CN/CdSe‐D) S‐scheme heterojunction synthesized using organic–inorganic hybrid approach employed for PHP first time. The optimization interface I K contributed to enhanced light absorption capabilities reduced interlayer transfer distance. Concurrently, synergy C─Se bonds at effectively modulated electron pathways. coordination environment mechanism are thoroughly investigated extended X‐ray fine structure in situ irradiated photoelectron spectroscopy. rate 40%K ‐CN/CdSe‐D reached 2240.23 µmol h −1 g pure water. This study highlights significance dual tuning chemical ionic intercalation effective strategy enhancing , paving way further advancements technology.

Язык: Английский

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