Enhancing Photosynthesis Efficiency of Hydrogen Peroxide by Modulating Side Chains to Facilitate Water Oxidation at Low‐Energy Barrier Sites DOI

Huijie Yan,

Peng Yuan, Yuyan Huang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(18)

Published: Jan. 27, 2024

Abstract Hydrogen peroxide (H 2 O ) is a crucial oxidant in advanced oxidation processes. In situ, photosynthesis of it natural water holds the promise practical application for remediation. However, current H systems primarily relies on oxygen reduction, leading to limited performance with low dissolved or anaerobic conditions found polluted water. Herein, novel photocatalyst based conjugated polymers alternating electron donor–acceptor structures and electron‐withdrawing side chains donors introduced. Specifically, carbazole functions as donor, triazine serves acceptor, cyano acts chain. Notably, exhibits remarkable solar‐to‐chemical conversion 0.64%, highest reported Furthermore, even conditions, achieves an impressive photosynthetic efficiency 1365 µmol g −1 h , surpassing all . This improvement attributed effective relocation active site from high‐energy low‐energy acetylene mediated by chains, resulting enhanced generation breakthrough offers new avenue efficient remediation using technologies oxygen‐limited environments, holding significant implications environmental restoration.

Language: Английский

Linkage-engineered donor–acceptor covalent organic frameworks for optimal photosynthesis of hydrogen peroxide from water and air DOI
Ruoyang Liu, Yongzhi Chen, Hongde Yu

et al.

Nature Catalysis, Journal Year: 2024, Volume and Issue: 7(2), P. 195 - 206

Published: Feb. 13, 2024

Language: Английский

Citations

146

Synergistic Effect of Oxygen Vacancy and High Porosity of Nano MIL‐125(Ti) for Enhanced Photocatalytic Nitrogen Fixation DOI Open Access
Yangyang Sun,

Houqiang Ji,

Yanjun Sun

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(3)

Published: Dec. 5, 2023

This work reports that a low-temperature thermal calcination strategy was adopted to modulate the electronic structure and attain an abundance of surface-active sites while maintaining crystal morphology. All experiments demonstrate new photocatalyst nano MIL-125(Ti)-250 obtained by has abundant Ti

Language: Английский

Citations

68

Recent progress and challenges of photocatalytic CO2 conversion into value-added multi-carbon products DOI
Chunmei Li, Jilong Wang, Lei Tong

et al.

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 502, P. 215623 - 215623

Published: Dec. 27, 2023

Language: Английский

Citations

53

Synergistic Effect of Oxygen Vacancy and High Porosity of Nano MIL‐125(Ti) for Enhanced Photocatalytic Nitrogen Fixation DOI Open Access
Yangyang Sun,

Houqiang Ji,

Yanjun Sun

et al.

Angewandte Chemie, Journal Year: 2023, Volume and Issue: 136(3)

Published: Dec. 5, 2023

Abstract This work reports that a low‐temperature thermal calcination strategy was adopted to modulate the electronic structure and attain an abundance of surface‐active sites while maintaining crystal morphology. All experiments demonstrate new photocatalyst nano MIL‐125(Ti)‐250 obtained by has abundant Ti 3+ induced oxygen vacancies high specific surface area. facilitates adsorption activation N 2 molecules on active in photocatalytic nitrogen fixation. The NH 3 yield over is enhanced 156.9 μmol g −1 h , twice higher than parent MIL‐125(Ti) (76.2 ). Combined with density function theory (DFT), it shows pattern tends be from “end‐on” “side‐on” mode, which thermodynamically favourable. Moreover, electrochemical tests atomic ratio /Ti 4+ can enhance carrier separation, also promotes efficiency may offer insights into design innovative photocatalysts for various chemical reduction reactions.

Language: Английский

Citations

52

Crystalline carbon nitrides for photocatalysis DOI Creative Commons
Han Li, Bei Cheng, Jingsan Xu

et al.

EES 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

39

Spaced Double Hydrogen Bonding in an Imidazole Poly Ionic Liquid Composite for Highly Efficient and Selective Photocatalytic Air Reductive H2O2 Synthesis DOI
Yu Cheng, Jie Jin, Huan Yan

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 15, 2024

Abstract Photocatalytic oxygen reductive H 2 O production is a promising approach to alternative industrial anthraquinone processes while suffering from the requirement of pure feedstock for practical application. Herein, we report spaced double hydrogen bond (IC−H‐bond) through multi‐component Radziszewski reaction in an imidazole poly‐ionic‐liquid composite (SI‐PIL‐TiO ) and levofloxacin hydrochloride (LEV) electron donor highly efficient selective photocatalytic air production. It found that IC−H‐bond formed by imino (−NH−) group SI‐PIL‐TiO carbonyl (−C=O) LEV can switch active sites characteristic covered state fully exposed one shield strong adsorption N air, propel intenser positive potential more orbitals binding patterns surface establish competitive selectivity chemisorption. Moreover, high enrichment as site 2e − reduction ensures rapid . Therefore, enables total utilization conversion efficiency 94.8 % direct reduction, achieving rate 1518 μmol/g/h 16 23 times compared without groups (PIL‐TiO TiO , respectively.

Language: Английский

Citations

39

Boosting the photosynthesis of hydrogen peroxide directly from pure water and air over S-scheme fiber heterojunction DOI Open Access
Ke Li,

Junlun Mei,

Jingping Li

et al.

Science China Materials, Journal Year: 2024, Volume and Issue: 67(2), P. 484 - 492

Published: Jan. 12, 2024

Language: Английский

Citations

37

Rationally Designed Cyclooctatetrathiophene‐Based Porous Aromatic Frameworks (COTh‐PAFs) for Efficient Photocatalytic Hydrogen Peroxide Production DOI

Linzhu Cao,

Cong Wang, He Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: March 7, 2024

Constructing stable and efficient photocatalysts for H

Language: Английский

Citations

35

Regulating the H2O2 Photosynthetic Activity of Covalent Organic Frameworks through Linkage Orientation DOI
Jieyu Yue,

Li-Ping Song,

Zi‐Xian Pan

et al.

ACS 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

Innovative Conversion Strategy for Wastewater with One‐Pot Uranium Extraction and Valuable Chemical Production by a Smart COF Photocatalyst DOI

Liecheng Guo,

Yuting Yang,

Lele Gong

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: March 15, 2024

Abstract Environmental protection and resource reclamation make the extraction of uranium from uranium‐containing wastewater be a key role in nuclear chemistry industry. Although previous studies have revealed several effective methods materials for such use, however, few are concerned about discharge issues. In fact, direct treated into environment is still not green way. Here, an innovative conversion approach shown, which can simultaneously achieve to valuable chemical. This concept implemented by azobenzene‐pendent covalent organic framework, showing smart trans ‐to‐ cis photoresponsive properties both space electronic structure consequently, largely enhanced efficiency under UV irradiation, relative visible light irradiation. real wastewater, material found give selective 100% H 2 O generation (1872.3 µmol g −1 h ). The mechanism due unique photocatalysis coupling between reduction reaction (URR), aiming at recovery or removal, water oxidation (WOR), targeting chemical .

Language: Английский

Citations

35