Precise Single‐Atom Modification of Hybrid Lead Chlorides for Electron Donor‐Acceptor Effect and Enhanced Photocatalytic Aerobic Oxidation DOI

Yukong Li,

Ziyi Wang,

Yilin Jiang

et al.

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

Published: Oct. 25, 2024

Abstract Hybrid lead halides show significant potential in photocatalysis due to their excellent photophysical properties, but the atomically precise modification of organic component achieve synergistic interactions with halide units remains a great challenge. Herein, for first time, we have employed crystal engineering strategy construct class single‐atom‐substituted hybrid electron donor‐acceptor (D‐A) effect. The frameworks consist 1D linear [PbCl] + chains as inorganic building and benzoxadiazole/benzothiadiazole/ benzoselenadiazole‐funtionalized dicarboxylates linkers. covalent bonding between ligands electron−withdrawing groups electron‐rich not only facilitate charge separation, also enhance structural robustness that is critical photocatalysis. D‐A structured serve highly efficient heterogeneous photooxidation catalysts, including aerobic oxidation C(sp 3 )−H bonds, oxidative coupling primary amines, phenylboronic acids selective sulfides are demonstrated 30 examples. Importantly, these reactions able be driven by natural sunlight ambient air afford quantitative yields. Moreover, our photocatalysts successful fix into photocatalytic flow system, which enables flow‐type synthesis high value‐added products on gram scale.

Language: Английский

Fully Conjugated Benzobisoxazole‐Bridged Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution DOI Open Access
Si Ma, Zhongping Li,

Yuxin Hou

et al.

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 6, 2025

Abstract 2D covalent organic frameworks (2D‐COFs) have attracted extensive interest in solar energy to hydrogen conversion. However, insufficient light harvesting and difficult exciton dissociation severely limit the improvement of photocatalytic activity for COFs, thereby impeding progression this advanced field. In work, two benzobisoxazole‐bridged fully conjugated 2D‐COFs with triazine (COF‐JLU44) pyrene (COF‐JLU45) units were constructed first time via Knoevenagel polycondensation, they hold long‐range ordered structures, largely acceptable surface area, fascinating photoelectric properties. Significantly, COF‐JLU45 exhibits an impressive evolution rate 272.5 mmol g −1 h superior reusability presence 1.0 wt% Pt under irradiation, coupled a remarkable apparent quantum yield 12.9% at long wavelength 600 nm. Multiple spectroscopy theoretical simulation demonstrate ingenious design widen its absorption effectively promote dissociation. This finding contributes valuable insights constructing metal‐free photocatalysts conversion utilization.

Language: Английский

Citations

0
In Situ Halide Vacancy Tuning of Low‐Dimensional Lead Perovskites to Realize Multiple Adjustable Luminescence Performance DOI Creative Commons
Chen Sun,

Chang‐Qing Jing,

Dongyang Li

et al.

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

Published: March 17, 2025

Abstract Surface defects play a crucial role in the photophysical properties and optoelectronic applications of perovskite materials. Although luminescent efficiency is improved through post‐synthetic defect passivation, comprehensive optimization photoluminescent performance via chemistry remains significant challenge. Herein, successful engineering strategy demonstrated toward 0D [DADPA]PbBr 5 (DADPA = diaminodipropylamine) single crystal to achieve multiple adjustable properties. Through fine‐tuning crystallization environment diminish Br vacancy ( V ), displays gradually evolutionary luminescence range from broadband blue‐white narrow green light emissions, with continuously dominant wavelengths (445–535 nm) linewidths (134–27 nm). Meanwhile, quantum yields increase significantly 3.7% 80.8%, lifetime extends 5.4 57.7 ns. This pioneering discovery for simultaneous modification multi‐dimensional performances. Combined spectroscopic investigations first‐principles calculations indicate that reducing narrows bandgap inhibits nonradiative recombination, which attenuates interband trap‐state‐associated emission facilitates formation bound exciton enhanced efficiency. More remarkably, this universal can be extended other systems similar adjustability, paving way diverse perovskites performance.

Language: Английский

Citations

0
Cu doping induced asymmetric Cu-Vs-In active sites in In2S3 for efficient photocatalytic C2H4 conversion from CO2 DOI
Fangyuan Xing, Qingfeng Li, J Li

et al.

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 691, P. 137388 - 137388

Published: March 20, 2025

Language: Английский

Citations

0
Recent advancements in all-inorganic and organic-inorganic hybrid metal halide materials for photocatalytic CO2 reduction reaction DOI

R. -Q. Chen,

Chenyang Wang, Xu Zhang

et al.

Frontiers in Energy, Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

Language: Английский

Citations

0
Poly‐Phosphamide Catalyzed Visible‐Light‐Driven CH4 and Dark‐Phase‐Mediated Cyclic Carbonate Productions Utilizing CO2 DOI
Nidhi Kumari, Kaushik Das, Monika Chaudhary

et al.

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

Published: April 10, 2025

Abstract A poly‐phosphamide (POP) with a band gap of 2.8 eV is used for the photochemical conversion CO 2 into CH 4 and chemical organo‐epoxides cyclic carbonates. The Tauc plot Mott Schottky analyses indicate conduction potential at −1.49 V (vs NHE), much more negative than multi‐electron reduction lifetime photo‐excited electron found ns. On photoirradiation 420 nm light, POP in presence triethanolamine or ascorbic acid can selectively convert (≈99%) yield 4.6 mmol g −1 . visible‐light irradiation, drop charge‐transfer resistance (R ct ) an enhancement cathodic current further confirm photon‐harvesting efficiency POP. In situ, FTIR study identifies adsorption to possible reaction intermediate, like *‐CO, *‐CH OH. also behaves as catalyst carbonates under solvent‐free conditions 98% yield. After light‐phase dark‐phase reactions, be successfully recycled least five times without structural degradation. Herein, acts bi‐functional, recyclable polymeric organic material essential feedstocks mild conditions.

Language: Английский

Citations

0
Enhanced Active Sites and Optimized Reaction Intermediate Configuration in PbBiO2Br Photocatalyst for Boosting Photocatalytic CO2 Reduction DOI
Jinwei Luo, Xiangdong Xue, Qichang Zhang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125396 - 125396

Published: April 1, 2025

Language: Английский

Citations

0
Construction of N-doped copper metal–organic frameworks for promoting photocatalytic carbon dioxide reduction to ethylene DOI
Fan Guo,

Zong-Zheng He,

Peng Wang

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 13, 2024

Language: Английский

Citations

3
Boosted photocatalytic CO2 conversion of a Cs2AgBiBr6@Co3O4 composite with high activity and selectivity under low-concentration CO2 and natural sunlight DOI
Yuxuan Song, Xiaoman Li, Hong Li

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 363, P. 124816 - 124816

Published: Nov. 12, 2024

Language: Английский

Citations

3
Selective Photocatalytic Conversion of CO2 to Ethanol via Unsaturated Cu–O Domains DOI
Qiang Wang, Mingqi He, Pengxin Yang

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 22, 2024

Enhancing the selectivity of photocatalytic CO2 reduction to valuable multicarbon (C2+) products remains a significant challenge in green synthetic chemistry. Here, we present dual-center strategy for metal oxides that boosts photochemical conversion ethanol by regulating coordination number and oxygen sites. Notably, CuO catalysts rich low-coordinated Cu–O domains have achieved nearly perfect (96.9%), extraordinary durability (60 h), superior yield rate 30.5 μmol·g–1·h–1, surpassing performance many existing photocatalysts water vapor CO2. Density functional theory calculations operando spectroscopic results provide conclusive evidence tricoordinated copper (Cu3c) increases coverage key *CO species, while bicoordinated (O2c) controls migration thereby effectively reducing energy requirement dimerization into *OC–CO intermediates (ΔG*OC–CO = −0.56 eV) pathway. This work offers insights designing exhibit improved C2+ fuels.

Language: Английский

Citations

3
Structure‐Function Relationship of p‐Block Bismuth for Selective Photocatalytic CO2 Reduction DOI
Jingwei Li,

Tianci Xiang,

Xiang Liu

et al.

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

Published: May 29, 2024

Abstract Selective photocatalytic reduction of CO 2 to value‐added fuels, such as CH 4 , is highly desirable due its high mass‐energy density. Nevertheless, achieving selective with higher production yield on p ‐block materials hindered by non‐ideal adsorption *CHO key intermediate and an unclear structure‐function relationship. Herein, we unlock the reaction steps found a volcano‐type relationship for ‐to‐CH conversion gradual p‐ band center Bi element leading formation Bi‐oxygen vacancy heterosites. The selectivity also positive correlation energy *CHO. heterosites appropriate filled Bi‐6 orbital electrons (−0.64) enhance coupling between C‐2 orbitals, thereby resulting in (95.2 %) productivity (17.4 μmol g −1 h ) towards . Further studies indicate that synergistic effect reduces Gibbs free *CO‐*CHO process, activates C−H C=O bonds *CHO, facilitates enrichment photoexcited at active sites multielectron conversion. This work provides new perspective developing elements

Language: Английский

Citations

2