Enabling direct-growth route for highly efficient ethanol upgrading to long-chain alcohols in aqueous phase

Juwen Gu, Wanbing Gong, Qian Zhang, Ran Long, Jun Ma, Xinyu Wang, Jiawei Li, Jiayi Li, Yujian Fan, Xinqi Zheng, Songbai Qiu (), Tiejun Wang () and Yujie Xiong ()
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Juwen Gu: Guangdong University of Technology
Wanbing Gong: University of Science and Technology of China
Qian Zhang: Guangdong University of Technology
Ran Long: University of Science and Technology of China
Jun Ma: University of Science and Technology of China
Xinyu Wang: University of Science and Technology of China
Jiawei Li: University of Science and Technology of China
Jiayi Li: University of Science and Technology of China
Yujian Fan: Guangdong University of Technology
Xinqi Zheng: Guangdong University of Technology
Songbai Qiu: Guangdong University of Technology
Tiejun Wang: Guangdong University of Technology
Yujie Xiong: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Upgrading ethanol to long-chain alcohols (LAS, C6+OH) offers an attractive and sustainable approach to carbon neutrality. Yet it remains a grand challenge to achieve efficient carbon chain propagation, particularly with noble metal-free catalysts in aqueous phase, toward LAS production. Here we report an unconventional but effective strategy for designing highly efficient catalysts for ethanol upgrading to LAS, in which Ni catalytic sites are controllably exposed on surface through sulfur modification. The optimal catalyst exhibits the performance well exceeding previous reports, achieving ultrahigh LAS selectivity (15.2% C6OH and 59.0% C8+OH) at nearly complete ethanol conversion (99.1%). Our in situ characterizations, together with theoretical simulation, reveal that the selectively exposed Ni sites which offer strong adsorption for aldehydes but are inert for side reactions can effectively stabilize and enrich aldehyde intermediates, dramatically improving direct-growth probability toward LAS production. This work opens a new paradigm for designing high-performance non-noble metal catalysts for upgrading aqueous EtOH to LAS.

Date: 2023
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DOI: 10.1038/s41467-023-43773-3

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