4.6 Article

Stable and Recyclable Photocatalysts of CsPbBr3@MSNs Nanocomposites for Photoinduced Electron Transfer RAFT Polymerization

Journal

ACS ENERGY LETTERS
Volume 7, Issue 12, Pages 4389-4397

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.2c02293

Keywords

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Funding

  1. National Natural Science Foundation of China [52172153, 51802254]
  2. Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]

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This study introduces a photocatalytic reaction called photoinduced electron transfer reversible addition-fragmentation chain transfer (PET-RAFT) polymerization using a CsPbBr3@MSNs nanocomposite as the photocatalyst. The embedded CsPbBr3 nanocrystals in dendritic mesoporous silica nanospheres (MSNs) successfully initiate the polymerization reaction, and the reaction variables are controlled to achieve polymers with desired characteristics.
All-inorganic metal halide perovskite CsPbX3 (X = Cl, Br, I) nanocrystals (NCs) have demonstrated attractive optoelectronic characteristics. However, their photocatalytic properties are limited by their poor stability and easy recombination of photogenerated carriers. Herein, we introduced a CsPbBr3@MSNs nanocomposite (CsPbBr3NCs embedded in dendritic mesoporous silica nanospheres (MSNs)) as photocatalysts for photoinduced electron transfer reversible addition-fragmentation chain transfer (PET-RAFT) polymerization. The CsPbBr3 nanocrystals (-8.1 nm; PLAY of 62 +/- 2.1%) were embedded in dendritic MSNs using a nanoconfinement strategy. PET-RAFT polymerization was successfully initiated using the CsPbBr3@MSNs nanocomposite as the photocatalyst. Reaction variables, such as catalyst loading, monomer composition, and excitation light wavelengths, were varied to yield polymers with the desired control of molecular weight and dispersity as well as block copolymers with high chain-end fidelity. In addition, the perovskite-based photocatalysts could be readily separated and purified, which allowed effective and rapid recycling of the nanocomposites for multiple polymerization cycles.

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