Hydrogenation of CO2 to Light Olefins over ZnZrOx /SSZ-13

Siyu Chen; Jiachen Wang; Zhendong Feng; Yiming Jiang; Hanwen Hu; Yuanzhi Qu; Shan Tang; Zelong Li; Jiaxu Liu; Jijie Wang; Can Li

doi:10.1002/anie.202316874

Hydrogenation of CO₂ to Light Olefins over ZnZrO_x /SSZ-13

Angew Chem Int Ed Engl. 2024 Feb 19;63(8):e202316874. doi: 10.1002/anie.202316874. Epub 2024 Jan 18.

Authors

Siyu Chen^{1

2}, Jiachen Wang³, Zhendong Feng^{1

2}, Yiming Jiang^{1

2}, Hanwen Hu^{1

4}, Yuanzhi Qu^{1

2}, Shan Tang^{1

2}, Zelong Li⁵, Jiaxu Liu³, Jijie Wang¹, Can Li^{1

2}

Affiliations

¹ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, China.
² University of Chinese Academy of Sciences, Beijing, 101408, China.
³ Department of Catalytic Chemistry and Engineering, State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, Liaoning 116012, China.
⁴ Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian 361005, China.
⁵ Key Laboratory of Advanced Catalysis, Gansu Province, State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, Gansu 730000, China.

PMID: 38179842
DOI: 10.1002/anie.202316874

Abstract

Converting CO₂ to olefins is an ideal route to achieve carbon neutrality. However, selective hydrogenation to light olefins, especially single-component olefin, while reducing CH₄ formation remains a great challenge. Herein, we developed ZnZrO_x /SSZ-13 tandem catalyst for the highly selective hydrogenation of CO₂ to light olefins. This catalyst shows C₂ ⁼ -C₄ ⁼ and propylene selectivity up to 89.4 % and 52 %, respectively, while CH₄ is suppressed down to 2 %, and there is no obvious deactivation. It is demonstrated that the isolated moderate Brønsted acid sites (BAS) of SSZ-13 promotes the rapid conversion of intermediate species derived from ZnZrO_x , thereby enhancing the kinetic coupling of the reactions and inhibit the formation of alkanes and improve the light olefins selectivity. Besides, the weaker BAS of SSZ-13 promote the conversion of intermediates into aromatics with 4-6 methyl groups, which is conducive to the aromatics cycle. Accordingly, more propene can be obtained by elevating the Si/Al ratio of SSZ-13. This provides an efficient strategy for CO₂ hydrogenation to light olefins with high selectivity.

Keywords: CO2 Hydrogenation; Light Olefins; SSZ-13; Tandem Catalysis; ZnZrOx.

Abstract

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