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

*Corresponding author for this work

Research output: Contribution to journalArticle

1 Citation (Scopus)

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 languageEnglish (US)
Pages (from-to)1923-1930
Number of pages8
JournalACS Catalysis
Volume9
Issue number3
DOIs
StatePublished - Mar 1 2019

Fingerprint

Fructose
Cobalt
Coke
Crystals
Catalysts
Oxides
Sintering
Sugars
Calcination
Fermentation
Raman scattering
Energy dispersive spectroscopy
Catalyst activity
Productivity
Metals
Particle size
methyl lactate
cobalt oxide
Costs
Experiments

Keywords

  • biomass conversion
  • cobalt oxide clusters
  • methyl lactate
  • silicalite-1
  • sinter-resistance

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Yan, Yue ; Zhang, Zihao ; Bak, Seong Min ; Yao, Siyu ; Hu, Xiaobing ; Shadike, Zulipiya ; Do-Thanh, Chi Linh ; Zhang, Feng ; Chen, Hao ; Lyu, Xilei ; Chen, Kequan ; Zhu, Yimei ; Lu, Xiuyang ; Ouyang, Pingkai ; Fu, Jie ; Dai, Sheng. / Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate. In: ACS Catalysis. 2019 ; Vol. 9, No. 3. pp. 1923-1930.
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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.",
keywords = "biomass conversion, cobalt oxide clusters, methyl lactate, silicalite-1, sinter-resistance",
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",
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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

Confinement of Ultrasmall Cobalt Oxide Clusters within Silicalite-1 Crystals for Efficient Conversion of Fructose into Methyl Lactate. / Yan, Yue; Zhang, Zihao; Bak, Seong Min; Yao, Siyu; Hu, Xiaobing; Shadike, Zulipiya; Do-Thanh, Chi Linh; Zhang, Feng; Chen, Hao; Lyu, Xilei; Chen, Kequan; Zhu, Yimei; Lu, Xiuyang; Ouyang, Pingkai; Fu, Jie; Dai, Sheng.

In: ACS Catalysis, Vol. 9, No. 3, 01.03.2019, p. 1923-1930.

Research output: Contribution to journalArticle

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

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.

KW - biomass conversion

KW - cobalt oxide clusters

KW - methyl lactate

KW - silicalite-1

KW - sinter-resistance

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