Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate

Yue Yan; Zihao Zhang; Seong Min Bak; Siyu Yao; Xiaobing Hu; Zulipiya Shadike; Chi Linh Do-Thanh; Feng Zhang; Hao Chen; Xilei Lyu; Kequan Chen; Yimei Zhu; Xiuyang Lu; Pingkai Ouyang; Jie Fu; Sheng Dai

doi:10.1021/acscatal.8b03230

Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate

Yue Yan, Zihao Zhang, Seong Min Bak, Siyu Yao, Xiaobing Hu, Zulipiya Shadike, Chi Linh Do-Thanh, Feng Zhang, Hao Chen, Xilei Lyu, Kequan Chen, Yimei Zhu, Xiuyang Lu, Pingkai Ouyang, Jie Fu, Sheng Dai

Department of Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

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.

Original language	English
Pages (from-to)	1923-1930
Number of pages	8
Journal	ACS Catalysis
Volume	9
Issue number	3
DOIs	https://doi.org/10.1021/acscatal.8b03230
Publication status	Published - 2019 Mar 1

Bibliographical note

Funding 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.

Publisher Copyright:
© 2018 American Chemical Society.

All Science Journal Classification (ASJC) codes

Catalysis
Chemistry(all)

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Yan, Y., Zhang, Z., Bak, S. M., Yao, S., Hu, X., Shadike, Z., Do-Thanh, C. L., Zhang, F., Chen, H., Lyu, X., Chen, K., Zhu, Y., Lu, X., Ouyang, P., Fu, J., & Dai, S. (2019). Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate. ACS Catalysis, 9(3), 1923-1930. https://doi.org/10.1021/acscatal.8b03230

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title = "Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate",

abstract = " 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.",

author = "Yue Yan and Zihao Zhang and Bak, {Seong Min} and Siyu Yao and Xiaobing Hu and Zulipiya Shadike and Do-Thanh, {Chi Linh} and Feng Zhang and Hao Chen and Xilei Lyu and Kequan Chen and Yimei Zhu and Xiuyang Lu and Pingkai Ouyang and Jie Fu and Sheng Dai",

note = "Funding 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. Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

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doi = "10.1021/acscatal.8b03230",

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Yan, Y, Zhang, Z, Bak, SM, Yao, S, Hu, X, Shadike, Z, Do-Thanh, CL, Zhang, F, Chen, H, Lyu, X, Chen, K, Zhu, Y, Lu, X, Ouyang, P, Fu, J & Dai, S 2019, 'Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate', ACS Catalysis, vol. 9, no. 3, pp. 1923-1930. https://doi.org/10.1021/acscatal.8b03230

TY - JOUR

T1 - Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate

AU - Yan, Yue

AU - Zhang, Zihao

AU - Bak, Seong Min

AU - Yao, Siyu

AU - Hu, Xiaobing

AU - Shadike, Zulipiya

AU - Do-Thanh, Chi Linh

AU - Zhang, Feng

AU - Chen, Hao

AU - Lyu, Xilei

AU - Chen, Kequan

AU - Zhu, Yimei

AU - Lu, Xiuyang

AU - Ouyang, Pingkai

AU - Fu, Jie

AU - Dai, Sheng

N1 - Funding 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. Publisher Copyright: © 2018 American Chemical Society.

PY - 2019/3/1

Y1 - 2019/3/1

N2 - 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.

AB - 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.

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Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate

Abstract

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