Programmed Charge Transfer in Conjugated Polymers with Pendant Benzothiadiazole Acceptor for Simultaneous Photocatalytic H2O2 Production and Organic Synthesis DOI

Sizhe Li,

Rong Ma, Chuanjun Tu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 14, 2024

While being important candidate for heterogeneous photocatalyst, conjugated polymer typically exhibits random charge transfers between the alternating donor and acceptor units, which severely limits its catalytic efficiency. Herein, inspired by natural photosystem, concept of guiding migration to specific reaction sites is employed significantly boost photocatalytic performance linear polymers (LCPs) with pendant functional groups via creating programmed charge-transfer channels from backbone moiety. The benzothiadiazole, as revealed in both situ X-ray photoelectron spectroscopy (XPS) density theory (DFT) calculations, can act electron "reservoir" that aggregates electrons at active sites. Moreover, presence channels, evidenced transient absorption (TAS), accelerates transfer, preventing recombination holes. As a result, this elaborately-designed architecture, photogenerated move smoothly towards reduction sites, facilitating O

Language: Английский

Synergy of Ni single atoms and NiO nanoclusters in carbon nitride to create local charge polarization for enhanced CO2 photoreduction DOI
Lei Li, Xinyan Dai,

Chao Cheng

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160101 - 160101

Published: Feb. 1, 2025

Language: Английский

Citations

4
Accompanying Bi Clusters as Charge Mediators Effectively Enhance Synergetic Redox of Bi2Sn2O7/ZnIn2S4 S‐Scheme Heterostructure Composites DOI Open Access
Xing Liu, Yu-Chen Su, Yudong Li

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Abstract Achieving synergistic oxidation and reduction represents a significant challenge in the field of photocatalysis. In this study, hydrothermal/in situ construction Bi atom clusters within 2 Sn O 7 /ZnIn S 4 (BSO/ZIS) heterostructures is reported. These exhibit self‐accelerating charge‐transfer mechanisms facilitated by internal electric fields bonding bridges, resulting highly efficient light absorption capabilities. X‐ray photoelectron spectroscopy (XPS) Kelvin probe force microscopy (KPFM), as well theoretical calculations, indicate that canonical induction promotion electrons holes lowers activation energy CHO* generation, allowing simultaneous CO toluene over catalyst, enhances proton‐coupling electron‐transfer processes, unique reaction mechanism. The reactant, Bi‐Bi (B‐BSO/ZIS) heterostructure achieves rate to 726.3 µmol g −1 h (99.9% selectivity) benzaldehyde 2362.0 (98.0% selectivity), which increases activity 14.6 5.7 times compared pristine ZnIn . This study underscores significance modulating photocatalytic pathway through strategic selection metal reactants, contributing rational design photocatalysts for enhanced adsorption stabilization *H.

Language: Английский

Citations

2
Enhanced Photocatalytic Production of Hydrogen Peroxide by Covalent Triazine Frameworks with Stepwise Electron Transfer DOI
Hao Zhang, Wenxin Wei, Kai Chi

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 17654 - 17663

Published: Nov. 15, 2024

The photosynthesis of hydrogen peroxide (H2O2) from pure water and oxygen using metal-free photocatalysts offers a renewable approach to convert solar energy storable chemical energy. However, the efficiency H2O2 is often hindered by rapid recombination photogenerated charge carriers. Herein, we present an elegantly designed covalent triazine framework (CTF) photocatalyst, denoted as Ace-asy-CTF, with stepwise electron transfer pathway for highly efficient H2O2. Notably, Ace-asy-CTF possesses localized excited-state distribution that created weakly conjugated acetenyl units in asymmetric frameworks, revealed transient spectroscopies further supported theoretical calculations. Meanwhile, introduced also serve active sites reduction reaction (ORR). simultaneously enhanced two-step 2e– ORR result excellent yield 2594 μmol g–1 h–1, directly produced without requiring any sacrificial reagents. This work paves way development next-generation catalysts, providing feasible benchmark stable

Language: Английский

Citations

9
Electrochemical Sulfonylation/Cyclization of N-Alkenylacrylamides with Sodium Sulfinates or Sulfonyl Hydrazides DOI
Zhixian Yang,

Lu-Cai Ding,

Gui-Hong Yang

et al.

The Journal of Organic Chemistry, Journal Year: 2024, Volume and Issue: 89(15), P. 10660 - 10677

Published: July 18, 2024

Two general protocols for the regioselective electrochemically enabled sulfonylation cyclization of

Language: Английский

Citations

8
Augmenting donor–acceptor covalent triazine frameworks for enhancing photocatalytic selective oxidation of sulfides DOI
Siyu Zhang, Fulin Zhang, Bing Zeng

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125147 - 125147

Published: Feb. 1, 2025

Language: Английский

Citations

1
Modulating the Moderate d‐Band Center of Indium in InVO4 Nanobelts by Synergizing MnOx and Oxygen Vacancies for High‐Efficiency CO2 Photoreduction DOI
Lei Li,

Huanhuan Liu,

Tianqi Li

et al.

Small, Journal Year: 2024, Volume and Issue: 20(45)

Published: July 27, 2024

Abstract Modulating the electronic properties of transition metal sites in photocatalysts at atomic level is essential for achieving high‐activity carbon dioxide photoreduction (CO 2 PR). An strategy herein proposed to engineer In‐d‐band center InVO 4 by incorporating MnO x nanoparticles and oxygen vacancies (V O ) into holey nanobelts (MnO /V ‐InVO ), which synergistically modulates a moderate consequently leads high‐efficiency CO PR. The catalyst with optimized property exhibits single evolution rate up 145.3 µmol g −1 h monoxide (CO) product selectivity 92.6%, coming out front reported ‐based materials. It discovered that modulated favors interaction between In their intermediates, thereby improves thermodynamics kinetics PR‐to‐CO reaction. This work not only demonstrates effective engineering d orbital low‐coordination atoms promote PR, but also paves way application tuning d‐band develop catalysts.

Language: Английский

Citations

4
Efficient photocatalytic C(sp3)-H oxidation of ethylbenzene enhanced by photochromic Mo-doped BiOCl ultrathin nanosheets DOI

Derong Kong,

Guanfeng Ji, Yao Dou

et al.

Journal of Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 115987 - 115987

Published: Jan. 1, 2025

Language: Английский

Citations

0
Insight into the role of photochromic effect in photocatalytic oxidation of ethylbenzene over h-MoO3 hexagonal microprisms DOI

Yongli Qin,

Guanfeng Ji, Yun Zhang

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160562 - 160562

Published: Feb. 1, 2025

Language: Английский

Citations

0
A tribute to Professor Dr Kai A. I. Zhang: pioneering advances in metal‐free polymeric photocatalysis DOI Creative Commons
Bolormaa Bayarkhuu, Sunil Kumar, Jeehye Byun

et al.

Polymer International, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 28, 2025

Abstract Polymeric photocatalysts have emerged as promising alternatives to traditional metal‐based catalysts due their tunable properties, low cost and environmental friendliness. This review highlights the significant contributions of Professor Dr Kai A. I. Zhang in advancing field polymeric photocatalysis. By leveraging structural versatility polymers, Zhang's work has developed innovative strategies enhance light absorption, charge separation catalytic activity. The delves into fundamental principles underlying photocatalysis, including exciton generation, carrier dynamics surface reactions. It further explores design considerations for optimizing polymer structures achieve efficient photocatalytic performance. Key advancements synthesis characterization are discussed, along with applications various chemical transformations. pioneering opened up new avenues development sustainable systems, driving transition towards a greener future. © 2025 Society Chemical Industry.

Language: Английский

Citations

0
Selective Toluene Oxidation Using Sulfur‐Doped Polymeric Carbon Nitride Photocatalysts DOI Creative Commons

Bayan Abed,

Venugopala Rao Battula, Michael Volokh

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 27, 2025

Abstract Selective traditional oxidation of toluene to high‐value products like benzyl alcohol, benzaldehyde, and benzoic acid faces significant challenges due high dissociation energy requirements, harsh reaction conditions, complex product distributions. While photocatalysis using O 2 as an oxidant offers a green alternative, developing efficient durable photocatalysts for selective in both batch flow systems remains challenging. Here, sulfur‐doped polymeric carbon nitride (S‐CN) is demonstrated versatile photocatalyst oxidation, applicable powder form binder‐free panels across various reactor configurations solvents. Tuning S monomer content within supramolecular assemblies that serve S‐CN precursors, allows enhanced light absorption, optimized band positions, specific surface area, tailored structural properties the ensuing catalysts. The achieves selectivity, yielding ∼72% benzaldehyde ∼26% after 24 h. Mechanistic studies confirm concurrent reduction reactions occurring roles · − 1 . Extended time (48 h) enables production (73.4%) with minimal formation (<1%), demonstrating excellent control.

Language: Английский

Citations

0