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
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
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
Citations
85Angewandte 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
Citations
83Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 331, P. 122691 - 122691
Published: March 25, 2023
Language: Английский
Citations
80Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(23)
Published: March 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
Language: Английский
Citations
76Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 334, P. 122862 - 122862
Published: May 7, 2023
Language: Английский
Citations
70Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(21)
Published: Feb. 26, 2023
Abstract Harnessing solar energy to produce hydrogen peroxide (H 2 O ) from water O) and dioxygen (O via artificial photosynthesis is an attractive route. To achieve high solar‐to‐H conversion efficiency, herein, interfacial self‐assembly strategy adopted pattern mesoporous resorcinol‐formaldehyde resin (MRF) onto reduced graphene oxide (rGO) form sandwich‐structured rGO@MRF polymeric photocatalysts. The internal layer that mimics the electron transport chain of plant leaf, can effectively transfer electrons, promote two‐electron reduction . Moreover, channels mimic stomata, beneficially boost fluid velocity, enrichment , diffusion H Consequently, developed metal‐free material exceptional solar‐to‐chemical efficiency 1.23%. This ingenious interface engineering brings new opportunities for design efficient
Language: Английский
Citations
62ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(6), P. 8066 - 8075
Published: Feb. 1, 2023
Conversing oxygen (O2) to hydrogen peroxide (H2O2) driven by solar energy is a promising H2O2 onsite production route but often short of efficient and durable photocatalysts. Herein, strong π-π conjugate polycyclic aromatic benzene acetylene units have been constructed into new covalent organic frameworks (COFs) linked imine C═N bonding. These COFs demonstrated two-dimensional hexagonal crystalline with higher crystallinity larger surface area (>600 m2 g-1). Covalent benzene-acetylene possessed appropriate visible light-responsive band structure the suppressed charge recombination rate. The -OH groups on their enable them be weakly hydrophilic. As result, it served as high-performance photocatalysts for in water-benzyl alcohol (BA) two-phase system. It delivered rate 1240 μmol h-1 gcat-1 catalytic efficiency within 60 h, comparable best COF-based catalysts. This study provides an photocatalytic system based hydrophilic imine-linked
Language: Английский
Citations
55EnergyChem, Journal Year: 2023, Volume and Issue: 6(1), P. 100116 - 100116
Published: Nov. 29, 2023
Language: Английский
Citations
54EES Catalysis, Journal Year: 2024, Volume and Issue: 2(2), P. 411 - 447
Published: Jan. 1, 2024
This review comprehensively summarizes the recent advances on crystalline carbon nitrides, including their preparation, optimization strategies, photocatalytic applications, as well challenges and prospects.
Language: Английский
Citations
40ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(7), P. 4728 - 4737
Published: March 13, 2024
Imine-linked isomeric covalent organic frameworks (COFs) with opposite linkage orientations are not rare, but their structure and photocatalytic property corrections still puzzling, let alone the emerging photosynthetic H2O2 performance. Herein, a pair of COFs (TB-COF TA-COF) reversed imine linkages was fabricated. Compared to TA-COF, TB-COF exhibited larger dipole moments better charge carrier separation efficiency, resulting in superior photosynthesis capability via dominant oxygen reduction reaction (ORR) paths (O2–O2•––H2O2 O2–O2•––O21–H2O2) feeble water oxidation (WOR) paths. With no sacrificial agents air, rates were 5186 μmol g–1 h–1 4111 natural seawater, respectively. The seawater-produced can be directly utilized for tetracycline degradation, manifesting big picture wastewater treatment by H2O2. Theoretical calculations revealed that hydroxyl-rich benzene ring photooxidation part triazine unit primary photoreduction part. Through linkage-orientation regulation, electronic structures, migration property, energy barrier rate determination step 2e– ORR WOR well-modulated. current work provides insight into effect orientation on performance may enlighten design catalysts photosynthesis.
Language: Английский
Citations
35