Issue 6, 2024

Homogeneous-like photocatalysis: covalent immobilization of an iridium(III) complex onto polystyrene brushes grafted on SiO2 nanoparticles as a mass/charge transfer-enhanced platform

Abstract

Current heterogeneous photocatalysis faces the major bottlenecks of limited mass transfer, charge recombination and tedious immobilization of expensive photocatalysts. In this work, fac-Ir(ppy)3 is directly anchored at a low cost via covalent linkage to poly(4-vinyl benzyl chloride) (PVBC) brushes grafted on SiO2 nanoparticles (PVBC@SiO2 NPs) via Friedel–Crafts alkylation, affording PVBC@SiO2 NP-supported fac-Ir(ppy)3 with high luminous efficacies such as emission lifetime and quantum yield. In the reductive cross-coupling of benzaldehydes/acetophenones with 1,4-dicyanobenzene (1,4-DCB), the as-fabricated photocatalyst affords benzhydrols in the same yields as homogeneous fac-Ir(ppy)3, except for o-substituted benzaldehydes/acetophenones. In terms of the same yields as homogeneous fac-Ir(ppy)3, a new catalytic model, named homogeneous-like photocatalysis, is proposed. In this catalytic model, the open stretching of PVBC brushes in DMSO enables the anchored fac-Ir(ppy)3 to catalyse the reaction in a similar manner as homogeneous fac-Ir(ppy)3, effectively avoiding charge recombination and mass transfer limitation. Furthermore, no significant decrease in yield (<5%) is observed over eight catalytic cycles, due to the good chemical and mechanical stabilities of PVBC@SiO2 NP-supported fac-Ir(ppy)3. Overall, the immobilization of fac-Ir(ppy)3 onto the PVBC brushes grafted on SiO2 NPs provides a mass/charge transfer-enhanced platform for supported photocatalysts.

Graphical abstract: Homogeneous-like photocatalysis: covalent immobilization of an iridium(III) complex onto polystyrene brushes grafted on SiO2 nanoparticles as a mass/charge transfer-enhanced platform

Supplementary files

Article information

Article type
Paper
Submitted
21 Nov 2023
Accepted
03 Jan 2024
First published
05 Jan 2024

Dalton Trans., 2024,53, 2731-2740

Homogeneous-like photocatalysis: covalent immobilization of an iridium(III) complex onto polystyrene brushes grafted on SiO2 nanoparticles as a mass/charge transfer-enhanced platform

S. Chen, Y. Zhou and X. Ma, Dalton Trans., 2024, 53, 2731 DOI: 10.1039/D3DT03903J

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements