Keto-enol tautomerism as transformative electron/hole traps to promote charge carrier separation for record-high H2O2 photosynthesis in real world DOI Creative Commons
Tianyi Ma, Fang Ma, Xiaodong Sun

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 30, 2024

Abstract Covalent organic frameworks (COFs) are excellent photocatalysts for hydrogen peroxide (H2O2) photosynthesis, but often limited by retarded charge carrier separation. Presently, donor-acceptor (D-A) type COFs commonly used to enhance the separation of photogenerated electrons and holes at molecular level promoting migration towards acceptor movement donor. However, significantly slower kinetics synchronous water oxidation oxygen reduction reactions (WOR ORR) result in accumulation carriers, which induces strong Coulomb forces, turn adversely affecting efficiency D-A COFs. Herein, it is observed that keto-enol tautomerism can function as dynamic traps both holes, alternately capturing them, while counterpart participate consumed during asynchronous reactions. This represents first example T-C (T denotes units; C catalytic active units), effectively weaken force reducing accumulation, resulting rapid transfer prolonged lifetimes free carriers efficient alternating photocatalytic WOR ORR. Our in-depth research indicates imine based on 2,4,6-trihydroxybenzaldehyde-1,3,5-tricarbaldehyde (Tp series) exhibit enhanced activity compared those 1,3,5-benzenetricarboxaldehyde (BT series), be attributed occurrence tautomerization. Notably, optimal Tp COF (TpBpy) displays an ultrafast rate H2O2 reaching 3.79 mM h-1, surpassing all previously reported photocatalysts. More importantly, when employed a flow-reactor system, TpBpy also showcases exceptional effectiveness continuous synthesis, achieving solar-to-chemical conversion (SCC) 0.038%, representing highest performance recorded date under natural sunlight conditions. work offers molecular-level guidance designing photosynthesis proposes standardized criteria obtaining reliable SCC values.

Language: Английский

Design and Preparation of Heterostructured Cu2O/TiO2 Materials for Photocatalytic Applications DOI Creative Commons

Yating Tai,

Boxuan Yang, Jing Li

et al.

Molecules, Journal Year: 2024, Volume and Issue: 29(21), P. 5028 - 5028

Published: Oct. 24, 2024

The extensive use of fossil fuels has sped up the global development world economy and is accompanied by significant problems, such as energy shortages environmental pollution. Solar energy, an inexhaustible clean resource, emerged a promising sustainable alternative. Light irradiation can be transformed into electrical/chemical which used to remove pollutants or transform contaminants high-value-added chemicals through photocatalytic reactions. Therefore, photocatalysis strategy overcome increasing problems. As well-known, photocatalysts are key components systems. Among widely investigated photocatalysts, titanium dioxide (TiO

Language: Английский

Citations

4
Ni‐SPO‐Al Catalyzed Stereoselective C–H Alkenylation of Quinazolinones with Alkynes to Prepare trans‐Isomers DOI
Yaqi Zhang,

Qiang Ni,

Rihui Cao

et al.

European Journal of Organic Chemistry, Journal Year: 2025, Volume and Issue: 28(5)

Published: Jan. 4, 2025

Abstract A stereoselective Ni−Al bimetal‐catalyzed C−H alkenylation of quinazolinones with alkynes has been successfully developed. Good selectivity Z‐type quinazolinone products was obtained using readily available substrates, which exhibits a trans‐configuration opposite to the conventional alkynylation reactions and improves diversity compounds. In addition, reaction process further explored through KIE other control experiments, possible mechanism proposed.

Language: Английский

Citations

0
Palladium-Catalyzed Divergent Synthesis from o-Sulfonamido Trifluoroacetophenones and 2-En-4-ynyl Carbonates DOI

Meng-Qi Gan,

Jian‐Xiang Zhu,

Zhichao Chen

et al.

Organic Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 15, 2025

Here we present a palladium-catalyzed divergent transformative reaction between o-sulfonamido trifluoroacetophenones and 2-en-4-ynyl carbonates. A spectrum of enantioenriched 2,5-dihydrofuran-fused tetrahydroquinolines bearing either (Z)- or (E)-exocyclic double bond are constructed with moderate to high enantioselectivity from 5-aryl-substituted carbonates by tuning palladium sources, while analogous 2,3-dihydrofuran-fused products furnished using 5-alkyl-substituted ones.

Language: Английский

Citations

0
Stereodivergent Construction of Enamides via a Radical-Mediated Isodesmic Reaction DOI
Yingying Xu, Xin Zhang, X. Kang

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 6749 - 6759

Published: April 10, 2025

Language: Английский

Citations

0
A green Heck reaction protocol towards trisubstituted alkenes, versatile pharmaceutical intermediates DOI Creative Commons
Giacomo Rossino, Giorgio Marrubini, Margherita Brindisi

et al.

Frontiers in Chemistry, Journal Year: 2024, Volume and Issue: 12

Published: July 10, 2024

The Heck reaction is widely employed to build a variety of biologically relevant scaffolds and has been successfully implemented in the production active pharmaceutical ingredients (APIs). Typically, with terminal alkenes gives high yields stereoselectivity toward

Language: Английский

Citations

3
Enantiospecific 1,3-hydrogen transfer of alkenes and alkynes DOI
Qi Liu,

Wan-Yi Xu,

Cen-Cen You

et al.

Trends in Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 1, 2024

Language: Английский

Citations

2
Divergent Synthesis of Chiroptical Molecular Switches Based on 1,2-Diaxial Atropisomers DOI Creative Commons

Tian‐Jiao Han,

Qingxiang Yang, Jin‐Feng Hu

et al.

JACS Au, Journal Year: 2024, Volume and Issue: 4(11), P. 4445 - 4454

Published: Oct. 14, 2024

The development of chiroptical molecular switches for chiral sensing, data communication, optical displays, logic gates, and asymmetric catalysis is currently a vibrant frontier science technology. Herein, we report practical artificial dynamic system based on 1,2-diaxial atropisomer. Organocatalytic parallel kinetic resolution allows the divergent synthesis two sets stereoisomers with vicinal C-C N-N axes from same racemic single-axis substrates. By simply varying configuration single catalyst, all four are accessible. successive conduction covalent unlocking/locking thermal-isomerization processes enables sequential switching between atropisomeric states electronic circular dichroism signal reversal, providing an example multistate switches.

Language: Английский

Citations

2
Photoswitched Stereodivergent Synthesis of Allylic Sulfones DOI

Hua‐Shan Huang,

Liuhui Xu,

Chun-Mei Zhang

et al.

Organic Letters, Journal Year: 2024, Volume and Issue: 26(23), P. 4916 - 4920

Published: May 31, 2024

The present Letter demonstrates a photoswitched stereodivergent synthesis of allylic sulfones from sodium sulfinates, triphenylvinylphosphonium chloride, and (hetero)aromatic aldehydes in single step. Mechanistically,

Language: Английский

Citations

0
Photocatalytic Radical-Promoted Cyclization of Thiomethyl Ynones with Aldehydes: Synthesis of Thiochromones DOI
Peipei Ma, Lulu Xu, Hongli Wu

et al.

Published: Jan. 1, 2024

Language: Английский

Citations

0
Organocatalytic Atroposelective Synthesis of Axially Chiral Indolyl Ketosulfoxonium Ylides DOI Open Access
Ji‐Wei Zhang, Yichi Zhang, Yong Huang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 137(1)

Published: Aug. 6, 2024

Abstract Despite recent advancements in the catalytic generation of axial chirality, reports on non‐biaryl atropisomers remain limited because stringent steric requirements necessary to establish effective rotational brakes. Herein, we present a novel class monoaryl atropisomers, indolyl ketosulfoxonium ylides, and describe an organocatalytic protocol for their synthesis. We discovered that chiral phosphoric acid (CPA) serves as catalyst highly enantioselective iodination ortho ‐aminophenylethynyl sulfoxonium ylides. Under optimized reaction conditions, strong preference intended process over competing protonation was observed. Subsequently, intramolecular amide cyclization enabled formation sterically congested indole fragments. Furthermore, synthetic utility products demonstrated by showcasing versatile transformations into other scaffolds with complete retention optical purity.

Language: Английский

Citations

0