期刊
NANO LETTERS
卷 22, 期 20, 页码 8381-8388出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c03087
关键词
carbon-based catalyst; atomically dispersed dual metal sites; tandem catalysis; olefin epoxidation; CO2 utilization
类别
资金
- National Natural Science Foundation of China [22101288, 21876183, 21905295, 22179141]
- Zhejiang Provincial Natural Science Foundation of China [LQ22B010005, LY21B030006]
- Ningbo Yongjiang Talent Introduction Programme [2021A-036-B]
- Science and Technology Innovation 2025 Program in Ningbo [2019B10046, 2020Z059, 2020Z107]
- Ningbo Natural Science Foundation [2021J202]
- Hundred Talents Program in the Chinese Academy of Sciences
- Shanghai Rising-star Program [20QA1402400]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21000000]
- DNL Cooperation Fund, CAS [DNL202008]
- Feringa Nobel Prize Scientist Joint Research Center
This work demonstrates that a rationally synthesized carbon-based catalyst achieves superior catalytic activity for the oxidative carboxylation of olefins. The synergistic effect between Fe and Al sites contributes to the excellent catalytic performance, providing insights for the future design of multifunctional catalysts.
Tandem catalysis provides an economical and energy-efficient process for the production of fine chemicals. In this work, we demonstrate that a rationally synthesized carbon-based catalyst with atomically dispersed dual Fe-Al sites (ADD-Fe-Al) achieves superior catalytic activity for the one-pot oxidative carboxylation of olefins (conversion similar to 97%, selectivity similar to 91%), where the yield of target product over ADD-Fe-Al is at least 62% higher than that of monometallic counterparts. The kinetic results reveal that the excellent catalytic performance arises from the synergistic effect between Fe (oxidation site) and Al sites (cycloaddition site), where the efficient CO2 cycloaddition with epoxides in the presence of Al sites (3.91 wt %) positively shifts the oxidation equilibrium to olefin epoxidation over Fe sites (0.89 wt %). This work not only offers an advanced catalyst for oxidative carboxylation of olefins but also opens up an avenue for the rational design of multifunctional catalysts for tandem catalytic reactions in the future.
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