Ultra-Highly Active Ni-Doped MOF-5 Heterogeneous Catalysts for Ethylene Dimerization

Cailing Chen; Lingkun Meng; Mohammed R. Alalouni; Xinglong Dong; Zhi Peng Wu; Shouwei Zuo; Huabin Zhang

doi:10.1002/smll.202301235

Ultra-Highly Active Ni-Doped MOF-5 Heterogeneous Catalysts for Ethylene Dimerization

Cailing Chen^*, Lingkun Meng, Mohammed R. Alalouni, Xinglong Dong^*, Zhi Peng Wu, Shouwei Zuo, Huabin Zhang

^*Corresponding author for this work

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

19 Scopus citations

Abstract

Here, an ultra-highly active Ni-MOF-5 catalyst with high Ni loading for ethylene dimerization is reported. The Ni-MOF-5 catalysts are synthesized by a facile one-pot co-precipitation method at room temperature, where Ni²⁺ replaces Zn²⁺ in MOF-5. Unlike Zn²⁺ with tetrahedral coordination in MOF-5, Ni²⁺ is coordinated with extra solvent molecules except for four-oxygen from the framework. After removing coordinated solvent molecules, Ni-MOF-5 achieves an ethylene turnover frequency of 352 000 h⁻¹, corresponding to 9040 g of product per gram of catalyst per hour, at 35 °C and 50 bar, far exceeding the activities of all reported heterogeneous catalysts. The high Ni loading and full exposure structure account for the excellent catalytic performance. Isotope labeling experiments reveal that the catalytic process follows the Cossee–Arlman mechanism, rationalizing the high activity and selectivity of the catalyst. These results demonstrate that Ni-MOF-5 catalysts are very promising for industrial catalytic ethylene dimerization.

Original language	English (US)
Article number	2301235
Journal	Small
Volume	19
Issue number	25
DOIs	https://doi.org/10.1002/smll.202301235
State	Published - Jun 21 2023

Bibliographical note

Funding Information:
C.C. and L.M. contributed equally to this work. The authors thank Prof. Yu Han for his strong support and meaningful discussion. The financial support for this work was provided by Baseline Funds (BAS/1/1372‐01‐01) and Research Translation Funds (REI/1/4220‐01‐01) from King Abdullah University of Science and Technology (KAUST). The authors also thank Dr. Xueyin Bai for his helpful suggestions.

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

ethylene dimerization
heterogeneous catalysts
metal-organic frameworks
Ni-doping

ASJC Scopus subject areas

Biotechnology
General Chemistry
Biomaterials
General Materials Science
Engineering (miscellaneous)

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10.1002/smll.202301235

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title = "Ultra-Highly Active Ni-Doped MOF-5 Heterogeneous Catalysts for Ethylene Dimerization",

abstract = "Here, an ultra-highly active Ni-MOF-5 catalyst with high Ni loading for ethylene dimerization is reported. The Ni-MOF-5 catalysts are synthesized by a facile one-pot co-precipitation method at room temperature, where Ni2+ replaces Zn2+ in MOF-5. Unlike Zn2+ with tetrahedral coordination in MOF-5, Ni2+ is coordinated with extra solvent molecules except for four-oxygen from the framework. After removing coordinated solvent molecules, Ni-MOF-5 achieves an ethylene turnover frequency of 352 000 h−1, corresponding to 9040 g of product per gram of catalyst per hour, at 35 °C and 50 bar, far exceeding the activities of all reported heterogeneous catalysts. The high Ni loading and full exposure structure account for the excellent catalytic performance. Isotope labeling experiments reveal that the catalytic process follows the Cossee–Arlman mechanism, rationalizing the high activity and selectivity of the catalyst. These results demonstrate that Ni-MOF-5 catalysts are very promising for industrial catalytic ethylene dimerization.",

keywords = "ethylene dimerization, heterogeneous catalysts, metal-organic frameworks, Ni-doping",

author = "Cailing Chen and Lingkun Meng and Alalouni, {Mohammed R.} and Xinglong Dong and Wu, {Zhi Peng} and Shouwei Zuo and Huabin Zhang",

note = "Funding Information: C.C. and L.M. contributed equally to this work. The authors thank Prof. Yu Han for his strong support and meaningful discussion. The financial support for this work was provided by Baseline Funds (BAS/1/1372‐01‐01) and Research Translation Funds (REI/1/4220‐01‐01) from King Abdullah University of Science and Technology (KAUST). The authors also thank Dr. Xueyin Bai for his helpful suggestions. Publisher Copyright: {\textcopyright} 2023 Wiley-VCH GmbH.",

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AU - Chen, Cailing

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AU - Wu, Zhi Peng

AU - Zuo, Shouwei

AU - Zhang, Huabin

N1 - Funding Information: C.C. and L.M. contributed equally to this work. The authors thank Prof. Yu Han for his strong support and meaningful discussion. The financial support for this work was provided by Baseline Funds (BAS/1/1372‐01‐01) and Research Translation Funds (REI/1/4220‐01‐01) from King Abdullah University of Science and Technology (KAUST). The authors also thank Dr. Xueyin Bai for his helpful suggestions. Publisher Copyright: © 2023 Wiley-VCH GmbH.

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N2 - Here, an ultra-highly active Ni-MOF-5 catalyst with high Ni loading for ethylene dimerization is reported. The Ni-MOF-5 catalysts are synthesized by a facile one-pot co-precipitation method at room temperature, where Ni2+ replaces Zn2+ in MOF-5. Unlike Zn2+ with tetrahedral coordination in MOF-5, Ni2+ is coordinated with extra solvent molecules except for four-oxygen from the framework. After removing coordinated solvent molecules, Ni-MOF-5 achieves an ethylene turnover frequency of 352 000 h−1, corresponding to 9040 g of product per gram of catalyst per hour, at 35 °C and 50 bar, far exceeding the activities of all reported heterogeneous catalysts. The high Ni loading and full exposure structure account for the excellent catalytic performance. Isotope labeling experiments reveal that the catalytic process follows the Cossee–Arlman mechanism, rationalizing the high activity and selectivity of the catalyst. These results demonstrate that Ni-MOF-5 catalysts are very promising for industrial catalytic ethylene dimerization.

AB - Here, an ultra-highly active Ni-MOF-5 catalyst with high Ni loading for ethylene dimerization is reported. The Ni-MOF-5 catalysts are synthesized by a facile one-pot co-precipitation method at room temperature, where Ni2+ replaces Zn2+ in MOF-5. Unlike Zn2+ with tetrahedral coordination in MOF-5, Ni2+ is coordinated with extra solvent molecules except for four-oxygen from the framework. After removing coordinated solvent molecules, Ni-MOF-5 achieves an ethylene turnover frequency of 352 000 h−1, corresponding to 9040 g of product per gram of catalyst per hour, at 35 °C and 50 bar, far exceeding the activities of all reported heterogeneous catalysts. The high Ni loading and full exposure structure account for the excellent catalytic performance. Isotope labeling experiments reveal that the catalytic process follows the Cossee–Arlman mechanism, rationalizing the high activity and selectivity of the catalyst. These results demonstrate that Ni-MOF-5 catalysts are very promising for industrial catalytic ethylene dimerization.

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KW - metal-organic frameworks

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Ultra-Highly Active Ni-Doped MOF-5 Heterogeneous Catalysts for Ethylene Dimerization

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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