Direct synthesis of extra-heavy olefins from carbon monoxide and water

Chuanhao Wang; Junjie Du; Lin Zeng; Zhongling Li; Yizhou Dai; Xu Li; Zijun Peng; Wenlong Wu; Hongliang Li; Jie Zeng

doi:10.1038/s41467-023-37599-2

Direct synthesis of extra-heavy olefins from carbon monoxide and water

Nat Commun. 2023 Apr 3;14(1):1857. doi: 10.1038/s41467-023-37599-2.

Authors

Chuanhao Wang^#¹, Junjie Du^#¹, Lin Zeng¹, Zhongling Li¹, Yizhou Dai¹, Xu Li¹, Zijun Peng¹, Wenlong Wu¹, Hongliang Li², Jie Zeng^{3

4}

Affiliations

¹ Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China.
² Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China. lihl@ustc.edu.cn.
³ Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China. zengj@ustc.edu.cn.
⁴ School of Chemistry & Chemical Engineering, Anhui University of Technology, 243002, Ma'anshan, Anhui, P. R. China. zengj@ustc.edu.cn.

^# Contributed equally.

Abstract

Extra-heavy olefins (C₁₂₊⁼), feedstocks to synthesize a wide range of value-added products, are conventionally generated from fossil resources via energy-intensive wax cracking or multi-step processes. Fischer-Tropsch synthesis with sustainably obtained syngas as feed-in provides a potential way to produce C₁₂₊⁼, though there is a trade-off between enhancing C-C coupling and suppressing further hydrogenation of olefins. Herein, we achieve selective production of C₁₂₊⁼ via the overall conversion of CO and water, denoted as Kölbel-Engelhardt synthesis (KES), in polyethylene glycol (PEG) over a mixture of Pt/Mo₂N and Ru particles. KES provides a continuously high CO/H₂ ratio, thermodynamically favoring chain propagation and olefin formation. PEG serves as a selective extraction agent to hinder hydrogenation of olefins. Under an optimal condition, the yield ratio of CO₂ to hydrocarbons reaches the theoretical minimum, and the C₁₂₊⁼ yield reaches its maximum of 1.79 mmol with a selectivity (among hydrocarbons) of as high as 40.4%.

Abstract

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