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

Nb2C MXene quantum dots modulate built-in electric field within heterostructures for efficient solar-to-H2O2 conversion from seawater DOI

Yamei Huang,

Xinglin Wang, Huihui Zhang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125262 - 125262

Published: March 1, 2025

Language: Английский

Citations

0

Functional Groups‐Regulated Organic Semiconductors for Efficient Artificial Photosynthesis of Hydrogen Peroxide DOI Open Access
Xiaohui Yu, Zhen Wei, Yuan Qin

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 18, 2025

Abstract Hydrogen peroxide (H 2 O ) is an environmentally friendly reagent, and organic semiconductors (OSCs) are ideal photocatalysts for the synthesis of H due to their well‐defined molecular structure, strong donor‐acceptor interactions, efficient charge separation. This review discusses regulatory mechanisms functional group modifications in tuning photocatalytic performance OSCs, highlighting relationship between structure catalytic performance. For example, electron‐regulating groups, such as cyano halogen, induce dipoles, facilitating migration photogenerated electrons. Fluorine groups optimize band prolong carrier lifetime high electronegativity. π‐Conjugated extension like anthraquinone thiophene, expand conjugation, improve visible light capture, stabilize intermediates through redox cycles. Hydroxyl enhance surface hydrophilicity promote activation, while imine bond protonation adjusts distribution improves selectivity cycle stability. Multi‐active site sulfonic acid amide, accelerate reaction kinetics inhibit decomposition. Functional absorption, separation, reactions electronic regulation, intermediate adsorption optimization, proton‐electron transfer. Future work should integrate machine learning identify optimal combinations develop green functionalization strategies photocatalyst synthesis.

Language: Английский

Citations

0

Structural design and property regulation of organic polymers for photocatalytic synthesis of H2O2 DOI Creative Commons
Mingyang Xu,

Rongchen Shen,

Y. L. Mo

et al.

InfoScience., Journal Year: 2025, Volume and Issue: unknown

Published: April 21, 2025

Abstract Hydrogen peroxide (H 2 O ), an environmentally benign oxidizer, finds extensive applications in pulp bleaching, wastewater treatment, and medical sterilization. Photocatalytic H synthesis via water oxygen activation on semiconductor surfaces presents a sustainable production strategy. Notably, structurally tunable organic photocatalysts have emerged as promising candidates, which targeted molecular engineering can boost the photocatalytic performance by enlarging specific surface areas, extending light absorption ranges, facilitating charge carrier transport‐separation dynamics. Given growing significance of synthesis, comprehensive review this field has become imperative. This paper offers systematic examination visible‐light‐driven using various photocatalysts, including graphitic carbon nitride (g‐C 3 N 4 resorcinol‐formaldehyde (RF) resin, covalent frameworks (COFs), linear conjugated polymers (LCPs). The focus lies fundamental mechanistic elucidation, design reaction pathways active sites, modification strategies, establishment efficient systems. Extensive studies correlated efficiency with interfacial electron transfer kinetics spatial separation. Therefore, we methodically analyze key determinants governing photogenerated dynamics present strategies for enhancement. Furthermore, discuss emerging application scenarios enabled generation. Importantly, critically evaluates persistent challenges cutting‐edge solutions visible‐light‐mediated ultimately providing principles developing high‐efficiency photocatalysts.

Language: Английский

Citations

0

The Preparation of Arac-Cu Nanozyme Hydrogel with Polyphenol Oxidase-like Activity for the Rapid Detection of Tea Polyphenol DOI
Jie Li,

Zhichun Bi,

Yu Ma

et al.

Journal of Food Composition and Analysis, Journal Year: 2025, Volume and Issue: unknown, P. 107690 - 107690

Published: April 1, 2025

Language: Английский

Citations

0

Alkali metal cation adsorption–induced surface polarization in polymeric carbon nitride for enhanced photocatalytic hydrogen peroxide production DOI
Lijun Hu, Yimeng Du, Rui Liu

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 679, P. 456 - 464

Published: Oct. 2, 2024

Language: Английский

Citations

2

Donor Substitution Engineering of Hemicyanine Nanoparticles to Reprogram the Tumor Microenvironment and Enhance Fn14‐Targeted BiTE for Glioblastoma Photoimmunotherapy DOI

Gaowei Li,

Shichao Jiang, Zongliang Zhang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 5, 2024

Abstract Glioblastoma (GBM) is a highly malignant intracranial tumor with limited treatment options. Bispecific T‐cell engagers (BiTEs) are being explored for GBM treatment, but their success hindered by inadequate T cell infiltration and activation due to the acidic immunosuppressive microenvironment. Photothermal immunotherapy lyses tumors activates immune responses, complementing BiTEs. This study innovatively employs donor engineering strategy develop hemicyanine dyes (Hcys) that emit from near‐infrared (NIR) I NIR II. The Hcy excellent properties encapsulated in an amphiphilic micelle, forming nano assembly lactate oxidase (PLH1100). PLH1100 exhibits spectral absorption at 980 nm, photothermal conversion efficiency of 58.7%, capability NIR‐II imaging. Besides ablation, regulates lactic acid metabolism immunogenic death, improving microenvironment promoting activation. Further studies demonstrate effectively kills human murine cells, inhibits orthotopic U87 growth BALB/c‐nu mice, enhances efficacy Fn14‐targeted BiTE GL261 C57BL/6 achieving synergistic “1+1>2” therapeutic effect. Collectively, this work opens new pathway using Hcy‐based molecules combined drugs therapy, significant clinical potential.

Language: Английский

Citations

2

Integrated Cyano Groups into the Skeleton of Conjugated Polymers to Activate Molecular Oxygen for Boosting Photocatalytic H2O2 Efficiency DOI
Qing Wang,

Wenjiao Wang,

Liping Guo

et al.

ChemSusChem, Journal Year: 2024, Volume and Issue: unknown

Published: July 29, 2024

Abstract Conjugated polymers (CPs) have shown promising potential in the field of hydrogen peroxide (H 2 O ) photosynthesis. However, a deeper understanding interactions between building units and specific functional groups within molecular skeleton is necessary to elucidate mechanisms driving H generation. Herein, series typical donor‐acceptor (D‐A) conjugated (B‐B, B‐CN, B‐DCN) were synthesized by introducing different amounts cyano (‐CN) into skeleton. The strong electron withdrawing properties can greatly promote effective separation transfer photogenerated charges units, resulting an impressive efficiency generation (2128.5 μmol g −1 h for B‐DCN, representing 96‐fold enhancement compared B‐B. More importantly, experimental results theoretical calculations further revealed that introduction ‐CN markedly reduce adsorption energy (E ad , while serving as active site induce conversion crucial intermediate superoxide anions (⋅O − singlet oxygen ( 1 ), achieving dual‐channel (O →⋅O →H → ). This work provides valuable insights design efficient photosynthesis materials.

Language: Английский

Citations

1

Interface interaction modulates charge transfer in flower-like In2S3 nanosheets/COF composite for efficient solar-to-H2O2 conversion DOI
Yu Zhang,

Yamei Huang,

Xinglin Wang

et al.

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 358, P. 130374 - 130374

Published: Nov. 2, 2024

Language: Английский

Citations

1

Photocatalysis Without Borders: Charting Progress in Metal-Free Hydrogen Peroxide Synthesis DOI

Kapil Mohan Saini,

Kanika Solanki, Bhawna Kaushik

et al.

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(6), P. 114425 - 114425

Published: Oct. 18, 2024

Language: Английский

Citations

0

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

Sizhe Li,

Rong Ma, Chuanjun Tu

et al.

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

Published: Nov. 14, 2024

Abstract 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 2 into H , while remaining holes are directed oxidation centers, simultaneously oxidizing furfuryl alcohol furoic acid. optimized photocatalyst LCP‐BT demonstrates competitive productivity 868.3 μmol L −1 h (9.8 times higher than conventional LCP‐1) conversion over 95 % after 6 h.

Language: Английский

Citations

0