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Brönsted酸
ChemistrySelect · 2025 ·Vol. 10 ·期 15 ·e202501120 · IF 2

Compartmentalization of Brönsted Acid/Pybox-Ru(II) by Polymeric Micelles for One-Pot Tandem Catalysis

Peipei Ji,Xiuwu Wang,Lianpei Zhou,Guiyang Zhou,Tao Chen

Graphical This study develops polymeric micelles with Brönsted acid and pybox-Ru(II) catalysts encapsulated in hydrophobic cores for efficient one-pot tandem catalysis of deacetalization-transfer hydrogenation. The micelles, prepared via self-assembly of block copolymers, demonstrate excellent catalytic efficiency, offering a simple and effective strategy for tandem catalysis. One-pot tandem catalysis has been favored by researchers for its ability to achieve the advantage of a shortened production process. In this paper, polymeric micelles containing Brönsted acid/pybox-Ru(II) in the hydrophobic cores were prepared for one-pot tandem catalysis of deacetalization-transfer hydrogenation reaction. First, block copolymer P[NHS] 30 - b -P[PEG 2000 ] 68 containing activated ester (NHS) in the suspended chain was successfully synthesized by ring-opening metathesis polymerization (ROMP) using a functional monomer containing norbornene group (NB-NHS) and polyethylene glycol containing norbornene group (NB-PEG 2000 ) as the raw materials. Then, block copolymer P[COOH] 30 - b -P[PEG 2000 ] 68 containing Brönsted acid catalyst and complex P[pybox-Ru] 30 - b -P[PEG 2000 ] 68 containing pybox-Ru(II) catalyst were prepared by the activated ester functionalization strategy. The copolymers and complexes were characterized using nuclear magnetic resonance spectroscopy (NMR), X-ray photoelectron spectroscopy (XPS), and gel permeation chromatography (GPC). Then, polymeric micelles with the catalysts encapsulated in hydrophobic cores were achieved by the self-assembly of the above copolymers in water. The prepared polymeric micelles as catalytic nanoreactors were successfully applied to one-pot tandem catalysis of the deacetalization-transfer hydrogenation reaction, demonstrating excellent catalytic efficiency. This study provided a facile and efficient strategy for tandem catalysis.

研究领域: 化学工程 · 材料科学 · 催化化学
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CHINESE JOURNAL OF CATALYSIS · 2023 · IF 16.5

Ultrathin ZnTi-LDH nanosheet: A bifunctional Lewis and Brönsted acid photocatalyst for synthesis of N-benzylideneanilline via a tandem reaction

Cheng Liu,Mengning Chen,Yingzhang Shi,Zhiwen Wang,Wei Guo,Sen Lin,Jinhong Bi,Ling Wu

Two ultrathin ZnTi-LDH nanosheets with different thickness (1.4 and 4.0 nm) were prepared to study the interplay between the active site and catalytic performance in photocatalytic synthesis of N -benzylideneanilline via a tandem reaction. ZnTi-LDH nanosheet possesses dual isolated active sites including the coordinatively unsaturated Ti atoms (Lewis acid sites) and the H atoms of OH groups (Brönsted acid sites), achieving the activation of benzyl alcohol and nitrobenzene via C–O···Ti species and N–O···H–O species, respectively. Photogenerated holes and electrons facilitate the oxidation of benzyl alcohol to benzaldehyde and the reduction of nitrobenzene to aniline, respectively. The thinner sample possesses more active sites, facilitating not only the activation of reactants but also the separation of photogenerated carriers. Therefore, a thinner ZnTi-LDH nanosheet shows the high conversion (100%) and the high selectivity (96%). Finally, a synergetic photocatalytic mechanism connected to the molecular activation is illustrated at the molecule level.

研究领域: 材料科学 · 催化化学
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