Enhanced C(sp3)–H Selective Oxidation Using Efficient Polyoxometalate-Based Metal–Organic Framework Photocatalysts Synergized with Ir Metalloligands and Polyoxometalates DOI
Jing Wang,

Luoning Li,

Yanan Liu

et al.

Chemistry of Materials, Journal Year: 2024, Volume and Issue: 36(22), P. 11150 - 11159

Published: Nov. 9, 2024

Achieving efficient selective visible light-induced oxidation of benzyl C(sp3)–H to more valuable double-bonded compounds holds significant promise for organic synthesis. In this work, we fabricated an example Ir metalloligand-modified POMOF crystalline material, CI-SiW, which is noteworthy as the first POM immobilized in a MOF via coordination bonding. Under excitation light (10 W, λ = 410 nm), CI-SiW can catalyze isochromane with turnover number and frequency 954 1740 h–1, respectively. Excitingly, displays best TOF compared previous photocatalysts under same conditions, realizing maximum yield minimum amount photocatalyst. Furthermore, had good cyclic structural stability, 90.4% was still obtained after three reaction cycles.

Language: Английский

Zinc–Porphyrin Conjugated Polymer Nanosheets with Accelerated Charge Transfer Dynamics for Selective Photocatalytic CO2 Reduction to CH4 DOI
Jiaxin Wang, Shien Guo, Chao Xu

et al.

ACS Applied Nano Materials, Journal Year: 2025, Volume and Issue: 8(4), P. 2022 - 2032

Published: Jan. 22, 2025

The photocatalytic reduction of CO2 into methane has garnered significant attention; however, the multiple electron and proton processes involved in often result low products selectivity. Herein, we present a conjugated polymer photocatalyst (ZnTP-PDA), composed Zn-porphyrin pyrazine units, which effectively drives photoconversion to CH4. nanosheet structure ZnTP-PDA offers numerous absorption sites exposes catalytic active centers, thereby enhancing reaction kinetics. Experimental analyses theoretical calculations demonstrate that incorporated Zn improve adsorption capability charge separation efficiency, optimizing both kinetics thermodynamics, facilitating hydrogenation key intermediate *CO generate Consequently, exhibits an impressive CH4 generation rate 49.2 μmol h–1 selectivity 90.3% without use any photosensitizers, is approximately 17.6 times higher than pristine TP-PDA under visible light irradiation. This study underscores beneficial effects site engineering on photocatalysts tailoring product during reduction.

Language: Английский

Citations

1
Selective Preference of Pt Atoms on Covalent Triazine Frameworks in CO2 Photoreduction: Insight into Energy Transfer Mechanisms DOI
Shasha Liu, Chao Zhu, Chao Xu

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5694 - 5705

Published: March 24, 2025

Metal-loaded COF-based photocatalysts facilitate the conversion of CO2 and H2O into storable fuels through a photosynthesis-like mechanism, providing an efficient approach to addressing energy challenges. However, fundamental principles governing internal transfer reaction pathways remain insufficiently understood, posing significant barriers achieving photocatalytic reactions with high selectivity specificity. This study explores heavy-atom effect Pt on exciton-mediated by synthesizing single-atom dispersed PtSA-CTF nanoparticle-aggregated PtNP-CTF defective CTF substrates, thereby revealing selective preferences species their impact pathways. By combining exciton behavior characterization (fs-TA), photoreaction pathway validation (13CO2 isotope labeling) excited-state theoretical calculations (TD-DFT), it was demonstrated that excitons in undergo resonance intermediate during relaxation process from triplet state ground state. The *CO2 then reacts sequentially generated electrons protons, resulting performance CO yield 6.778 mmol·g–1·h–1, 98.2% selectivity, TOF 1102.68 h–1. work provides valuable insights photophysical properties induced excitonic effects, offering guidance for improving efficiency rational design advanced photocatalysts.

Language: Английский

Citations

0
Enhanced efficiency and selectivity in reactive oxygen species generation using thiazolo[5,4-d]thiazole-based supramolecular photosensitizers DOI
Guang Wang,

Tongfei Qi,

Xianjun Yin

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 21, 2025

Language: Английский

Citations

0
Developing multi-functional anthraquinone-based conjugated porous polymers for near-infrared-light-driven high selective cyanation of α-amino C(sp3)-H bonds DOI

Hong-Min Lin,

Xiaotong Li, Fei‐Hu Cui

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: April 8, 2025

Language: Английский

Citations

0
Photodegradation of PCB-209 on Suspended Particles: Discrepancy in Mechanism of Direct Dechlorination and Active Species-Mediated Indirect Dechlorination Reactions DOI
Jianqiao Xu, Xinyuan Wei,

Junyan Wei

et al.

Water Research, Journal Year: 2025, Volume and Issue: 283, P. 123797 - 123797

Published: May 9, 2025

Language: Английский

Citations

0
Pyrrole-Derived Covalent Organic Frameworks: A Promising Platform for Efficient Bifunctional Electrocatalytic Water Splitting DOI
Jinjian Wang, Zhenjie Lu,

Xiangyu Gao

et al.

ACS Applied Engineering Materials, Journal Year: 2025, Volume and Issue: unknown

Published: May 22, 2025

Language: Английский

Citations

0
A recyclable type‐I photosensitizer to enable red‐light‐driven gram‐scale aerobic photocatalysis DOI Creative Commons

Shirong Yan,

Lu Qiao, Lei Chen

et al.

Smart Molecules, Journal Year: 2025, Volume and Issue: unknown

Published: June 4, 2025

Abstract Developing metal‐free, purely organic photocatalysts with high recyclability and the ability to utilize red light yield specific reactive oxygen species for aerobic photocatalysis is both crucial challenging in current research. Herein, we first found that a type‐I photosensitizer, EtNBS‐H , can achieve red‐light‐driven remarkable catalytic performance facile recoverability. Upon irradiation light, exclusively generates O 2 −• enabling efficient hydroxylation of arylboronic acids, oxidization thioethers other substrates conversion exceeding 99%. Significantly, stands out its simple recovery reuse through pH‐tunable acid‐base reaction. This allows attainment high‐purity products extraction, enables retrieval photocatalyst from reaction medium subsequent an average rate 94%. Moreover, utilizing as scale‐up reaction, gram‐scale >95% purity >99% were obtained, highlighting potential guidance developing recyclable harness light. work offers promising approach sustainable large‐scale photocatalytic synthesis.

Language: Английский

Citations

0
Enhanced C(sp3)–H Selective Oxidation Using Efficient Polyoxometalate-Based Metal–Organic Framework Photocatalysts Synergized with Ir Metalloligands and Polyoxometalates DOI
Jing Wang,

Luoning Li,

Yanan Liu

et al.

Chemistry of Materials, Journal Year: 2024, Volume and Issue: 36(22), P. 11150 - 11159

Published: Nov. 9, 2024

Achieving efficient selective visible light-induced oxidation of benzyl C(sp3)–H to more valuable double-bonded compounds holds significant promise for organic synthesis. In this work, we fabricated an example Ir metalloligand-modified POMOF crystalline material, CI-SiW, which is noteworthy as the first POM immobilized in a MOF via coordination bonding. Under excitation light (10 W, λ = 410 nm), CI-SiW can catalyze isochromane with turnover number and frequency 954 1740 h–1, respectively. Excitingly, displays best TOF compared previous photocatalysts under same conditions, realizing maximum yield minimum amount photocatalyst. Furthermore, had good cyclic structural stability, 90.4% was still obtained after three reaction cycles.

Language: Английский

Citations

3