4.8 Article

Nanoparticle-Catalyzed Green Chemistry Synthesis of Polybenzoxazole

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 4, 页码 2115-2122

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c12488

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资金

  1. Office of Vice President of Research of Brown University
  2. Institute of Molecular and Nanoscale Innovation of Brown University
  3. National Science Foundation [1644760]
  4. Direct For Education and Human Resources
  5. Division Of Graduate Education [1644760] Funding Source: National Science Foundation

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Nanoparticle catalysts show promise in enabling multistep chemical reactions in a tandem fashion for green chemistry synthesis. Specifically, AuPd alloy NPs exhibit excellent catalytic performance in one-pot reactions to produce high-quality PBO, while Cu NPs can catalyze similar reactions to form PBO when formic acid is replaced.
Enabling catalysts to promote multistep chemical reactions in a tandem fashion is an exciting new direction for the green chemistry synthesis of materials. Nanoparticle (NP) catalysts are particularly well suited for tandem reactions due to the diverse surface-active sites they offer. Here, we report that AuPd alloy NPs, especially 3.7 nm Au42Pd58 NPs, catalyze one-pot reactions of formic acid, diisopropoxy-dinitrobenzene, and terephthalaldehyde, yielding a very pure thermoplastic rigid-rod polymer, polybenzoxazole (PBO), with a molecular weight that is tunable from 5.8 to 19.1 kDa. The PBO films are more resistant to hydrolysis and possess thermal and mechanical properties that are superior to those of commercial PBO, Zylon. Cu NPs are also active in catalyzing tandem reactions to form PBO when formic acid is replaced with ammonia borane. Our work demonstrates a general approach to the green chemistry synthesis of rigid-rod polymers as lightweight structural materials for broad thermomechanical applications.

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