Water-Promoted C–C Coupling Reaction in Plasma-Catalytic CO<sub>2</sub> Hydrogenation for Ethanol Production
The conversion of CO2 into alcohols has attracted widespread interest. Herein, we present an approach for the plasma-catalytic CO2 hydrogenation to ethanol over a Cu2O/CeO2 catalyst under atmospheric pressure at a low temperature of ∼75 °C. The Cu2O/CeO2 catalyst initially exhibits low ethanol selectivity (2.1%), which dramatically increases to 56% (78% total alcohols selectivity) with the assistance of water. D2O and H218O isotope-tracing experiments reveal the partial decomposition of water and the active involvement of its derivatives in the multistep pathway for ethanol synthesis. The multiple roles of H2O in switching alcohols production from methanol to ethanol are investigated. The plasma-generated OH in both adsorbed and radical states promotes C–C coupling via CO-H2CO bonding and facilitates hydrogenation through proton transfer. Additionally, the presence of adsorbed H2O and OH enhances the desorption of ethanol, further enhancing alcohol selectivity. It is envisaged that these findings would inspire value-added transformation of CO2 to produce higher alcohols and pave the way for efficient chemical processes.
Authors
- An‐Hui Lu (ORCID: https://orcid.org/0000-0003-1294-5928)
- Sara Bals (ORCID: https://orcid.org/0000-0002-4249-8017)
- Shengyan Meng (ORCID: https://orcid.org/0000-0001-9934-9314)
- Zhaolun Cui (ORCID: https://orcid.org/0000-0002-1027-1563)
- Yanhui Yi (ORCID: https://orcid.org/0000-0002-5869-9382)
- Dezheng Yang (ORCID: https://orcid.org/0000-0002-8549-3507)
- Erik C. Neyts (ORCID: https://orcid.org/0000-0002-3360-3196)
- Annemie Bogaerts (ORCID: https://orcid.org/0000-0001-9875-6460)
- Evgenii Vlasov (ORCID: https://orcid.org/0000-0003-3426-6248)
- Kellie Jenkinson (ORCID: https://orcid.org/0000-0002-1770-5678)
- Qian Chen (ORCID: https://orcid.org/0000-0002-2979-4866)
- Min Liu (ORCID: https://orcid.org/0000-0002-9007-4817)
- Hang Zhang (ORCID: https://orcid.org/0000-0001-5019-7209)
- Yi Liu (ORCID: https://orcid.org/0000-0002-2073-4832)
- Shangkun Li (ORCID: https://orcid.org/0000-0002-9297-1669)
Institutions
- Central South University (CN)
- University of Antwerp (BE)
- Dalian University of Technology (CN)
- Materials Modification (United States) (US)
- Powder Metallurgy Institute (BY)
- State Key Laboratory of Powder Metallurgy
- South China University of Technology (CN)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2025-02-07
- DOI
- https://doi.org/10.1021/acscatal.4c06543
- Citations
- 15
- Primary Topic
- Carbon dioxide utilization in catalysis
- Type
- article
- Field-Weighted Citation Impact
- 10.57
Funders
- National Natural Science Foundation of China
- Universiteit Antwerpen
- H2020 European Research Council
- H2020 Research Infrastructures