4.8 Article

Improved photocatalytic CO2 and epoxides cycloaddition via the synergistic effect of Lewis acidity and charge separation over Zn modified UiO-bpydc

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 301, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120793

关键词

CO2 cycloaddition; Lewis acidity; Carbon dioxide activation; Metal-organic frameworks; Photocatalysis

资金

  1. National Key Research and Development Program of China [2020YFA0710301]
  2. National Natural Science Foundation of China [U1832145, 22172088, 51972195, 21832005, 21972078, 11374190]
  3. Young Scholars Program of Shandong University [2020QNQT012]
  4. Shandong Province Natural Science Foundation [ZR2020YQ16]
  5. Taishan Scholar Foundation of Shandong Province, China

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The study explored the effects of Zn and Ce on the CO2 cycloaddition reaction, revealing that the introduction of Zn can effectively activate propylene oxide, promote LMCT process, while Ce plays a negative role under light irradiation, facilitating the energy transfer process.
CO2 cycloaddition reaction from propylene oxide and CO2 to cyclic carbonates is a desirable process to become carbon neutral. Photo energy can decrease the temperature and pressure needed for this reaction according to our previous results. However, the relationship between Lewis acidity and the photophysical process needs to be clarified and optimized. Hence, in this work, Zn is introduced into UiO-bpydc via the coordination of Zn with the bipyridyl group in bpydc. It is found that the introduction of Zn not only effectively activate propylene oxide, but also promote ligand to metal charge transfer (LMCT) process, which ultimately is beneficial for CO2 activation. However, Ce plays a negative effect under light irradiation. namely, the presence of Ce facilitates the energy transfer process rather than the LMCT process.

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