Boosted Photoreforming of Plastic Waste via Defect-Rich NiPS₃ Nanosheets

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(11), P. 6410 - 6419

Published: March 13, 2023

Sustainable conversion of plastic waste to mitigate environmental threats and reclaim value is important. Ambient-condition photoreforming practically attractive convert hydrogen (H2); however, it has poor performance because mutual constraint between proton reduction substrate oxidation. Here, we realize a cooperative photoredox using defect-rich chalcogenide nanosheet-coupled photocatalysts, e.g., d-NiPS3/CdS, give an ultrahigh H2 evolution ∼40 mmol gcat-1 h-1 organic acid yield up 78 μmol within 9 h, together with excellent stability beyond 100 h in commercial poly(lactic acid) poly(ethylene terephthalate). Significantly, these metrics represent one the most efficient reported. In situ ultrafast spectroscopic studies confirm charge transfer-mediated reaction mechanism which d-NiPS3 rapidly extracts electrons from CdS boost evolution, favoring hole-dominated oxidation improve overall efficiency. This work opens practical avenues for converting into fuels chemicals.

Language: Английский

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Enhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification

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

Published: April 13, 2024

Abstract Gold-based co-catalysts are a promising class of materials with potential applications in photocatalytic H 2 O production. However, current approaches Au show limited production due to intrinsically weak adsorption at the site. We report an approach strengthen sites, and improve production, through formation electron-deficient δ+ sites by modifying electronic structure. In this case, we synthesis TiO /MoS x -Au, following selective deposition onto MoS surface which is then further anchored . that catalyst achieves significantly increased rate 30.44 mmol g −1 h -saturated solution containing ethanol. Density functional theory calculations X-ray photoelectron spectroscopy analysis reveal mediator induces thereby decreasing antibonding-orbital occupancy Au-O ads subsequently enhancing adsorption. This strategy may be useful for rationally designing structure surfaces facilitate artificial photosynthesis.

Language: Английский

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Versatile Photoelectrocatalysis Strategy Raising Up the Green Production of Hydrogen Peroxide

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(14)

Published: March 1, 2023

Abstract H 2 O plays an irreplaceable role in many aspects of human society, such as paper bleaching, medical disinfection, wastewater treatment, organic synthesis, hydrometallurgy and the electronic industry. However, unsustainability current industrial production process traditional anthraquinone has a serious conflict with green sustainable development. The photo/electrocatalytic from renewable energy advantages being more economical, low‐carbon green, line requirements economy. These catalytic methods have played demonstrative development small molecules, contributing to fundamental understanding general catalysis providing scientific perspective for future new cycles. In this review, authors aim integrate reaction mechanism photocatalytic electrocatalytic production, summarize application recent years, assess modern technologies promoted research, including flux equipment coproduction, etc. This review intends provide clear logic profile directions calls researchers insights into field.

Language: Английский

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Photoredox‐Promoted Co‐Production of Dihydroisoquinoline and H₂O₂ over Defective Zn₃In₂S₆

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(10)

Published: Jan. 5, 2023

One of the most sustainable and promising approaches for hydrogen peroxide (H2 O2 ) production in a low-cost environment-friendly way is photosynthesis, which, however, suffers from poor carrier utilization low H2 productivity. The addition proton donors such as isopropanol or ethanol can increase production, unfortunately, will inevitably elevate entire cost while wasting oxidizing power holes (h+ ). Herein, tetrahydroisoquinolines (THIQs) employed distinctive donor thermodynamically feasible selective semi-dehydrogenation reaction to highly valuable dihydroisoquinolines (DHIQs), meanwhile, couple with promote generation one photoredox under photocatalysis by dual-functional Zn3 In2 S6 photocatalyst. Surprisingly, suitably defective offers an excellent near-stoichiometric co-production performance DHIQs at unprecedentedly high rates 66.4 62.1 mmol h-1 g-1 visible light (λ ≥ 400 nm), respectively, which outperforms all previously available reports even though sacrificial agents were those reports. Additionally, photocatalytic redox mechanism demonstrates that be generated through multiple pathways, highlighting synergistic effect among ROS (·O2- 1 ), h+ donor, has been ignored previous studies.

Language: Английский

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Highly crystalline carbon nitrogen polymer with a strong built-in electric fields for ultra-high photocatalytic H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123340 - 123340

Published: Sept. 26, 2023

Language: Английский

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Efficient sacrificial-agent-free solar H2O2 production over all-inorganic S-scheme composites

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 324, P. 122227 - 122227

Published: Nov. 26, 2022

Language: Английский

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Tailoring well-ordered, highly crystalline carbon nitride nanoarrays via molecular engineering for efficient photosynthesis of H2O2

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 317, P. 121723 - 121723

Published: July 8, 2022

Language: Английский

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The photocatalytic H2O2 production by metal-free photocatalysts under visible-light irradiation

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 341, P. 123271 - 123271

Published: Sept. 6, 2023

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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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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