期刊
CHEMICAL SCIENCE
卷 12, 期 11, 页码 3898-3910出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc05789d
关键词
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资金
- Center for Alkaline-based Energy Solutions (CABES), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0019445]
- National Institutes of Health [R35 GM134893]
- National Science Foundation (NSF) [CHE-1531632]
- NSF MRSEC [DMR-1719875]
- U.S. Department of Energy Office of Science User Facility [DE-AC02-05CH11231]
A novel method for preparing high-performance AAEMs through photocatalytic hydroamination reaction is reported in this study, addressing the challenges of complex synthesis of functionalized cyclooctene monomers, while also considering the importance of local backbone morphology in the rational design of stable high-performance AAEMs.
Alkaline anion exchange membranes (AAEMs) with high hydroxide conductivity and good alkaline stability are essential for the development of anion exchange membrane fuel cells to generate clean energy by converting renewable fuels to electricity. Polyethylene-based AAEMs with excellent properties can be prepared via sequential ring-opening metathesis polymerization (ROMP) and hydrogenation of cyclooctene derivatives. However, one of the major limitations of this approach is the complicated multi-step synthesis of functionalized cyclooctene monomers. Herein, we report that piperidinium-functionalized cyclooctene monomers can be easily prepared via the photocatalytic hydroamination of cyclooctadiene with piperidine in a one-pot, two-step process to produce high-performance AAEMs. Possible alkaline-degradation pathways of the resultant polymers were analyzed using spectroscopic analysis and dispersion-inclusive hybrid density functional theory (DFT) calculations. Quite interestingly, our theoretical calculations indicate that local backbone morphology-which can potentially change the Hofmann elimination reaction rate constant by more than four orders of magnitude-is another important consideration in the rational design of stable high-performance AAEMs.
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