Chemocatalysis of sugars to methyl lactate (MLA) exhibits great advantages over the conventional fermentation approach because of its higher productivity and cost-effective separation process. However, widely used supported metal oxide catalysts suffer from deactivation resulting from sintering during the reaction and removal of coke at high temperatures. Herein, we report ultrasmall cobalt oxide clusters (∼1.7 nm) stabilized within silicalite-1 crystals catalyst (CoO@silicalite-1), exhibiting superior catalytic activity and resistance to sintering for the conversion of fructose into methyl lactate. HAADF-STEM, EDS-mapping, and XRD experiments identify the existence of confined CoO clusters. XANES and Raman spectra demonstrated the covalent interaction between CoO and silicalite-1. Thanks to the ultrasmall CoO particle size (∼1.7 nm), the CoO@silicalite-1 affords nearly 100-fold higher Co-mass-based activity (mg MLA/mg Co) compared with CoO or Co 3 O 4 particles outside the silicalite-1 framework. More importantly, this catalyst exhibits good reuse performance via the removal of coke with facile calcination.
|Number of pages||8|
|Publication status||Published - 2019 Mar 1|
Bibliographical noteFunding Information:
This work was supported by the National Natural Science Foundation of China (Nos. 21436007, 21676243, 21706228), the Zhejiang Provincial Natural Science Foundation of China (No. LR17B060002), and the Fundamental Research Funds for the Central Universities (No. 2018QNA4038). S.D. was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Seongmin Bak and Zulipiya Shadike at Brookhaven National Laboratory were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract DE-SC0012704. The XAS research used beamline 8-ID of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704.
© 2018 American Chemical Society.
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