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Electrocatalytic CO2 hydrogenation to C2+ alcohols catalysed by Pr–Cu oxide heterointerfaces

Nature Synthesis volume 4, pages 730–743 (2025)Cite this article

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Abstract

Efficient production of C2+ alcohols from the electrochemical CO2 reduction reaction (CO2RR) is of great interest. However, the CO2RR to C2+ alcohols has low selectivity and current density due to competing C2+ pathways that produce ethylene (C2H4). Here we report a stepwise precipitation and stepwise calcination strategy to create Pr–Cu oxide heterointerfaces (Pr6O11–Cu-SS) that produces an efficient CO2RR to C2+ alcohols. Pr6O11–Cu-SS exhibited high productivity and Faradaic efficiency (FE) for C2+ alcohols. At −1.08 V versus RHE, the current density and FE of C2+ alcohols reached 700 mA cm−2 and 71.3%, respectively, with the FEs of ethanol and n-propanol reaching 58.6% and 12.7%, respectively, under these conditions. The C2+ alcohols/C2H4 ratio was as high as 12:1. Experimental and theoretical studies indicated that the performance of the catalyst results from the existence of a Pr4+/Pr3+ structure in Pr6O11–Cu-SS, which is able to effectively stabilize Cuδ+/Cu0 via a unique Pr–O–Cu linkage and form stable oxide heterointerfaces. The binding strength and binding type of *CO were then altered on the heterointerfaces to form a mixed adsorption configuration, which induces asymmetric carbon–carbon coupling and selective hydrodeoxygenation to promote the generation of C2+ alcohols.

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Fig. 1: Synthesis and electron microscopic analysis of the Pr6O11–Cu-SS catalyst.
Fig. 2: Electrochemical CO2RR performance.
Fig. 3: Spectroscopic characterization.
Fig. 4: Structural evolution of the Pr6O11–Cu-SS catalyst during the CO2RR.
Fig. 5: Mechanistic insight from DFT calculations.

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The data that support the findings of this study are available in the paper and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

The authors thank the National Key Research and Development Program of China (2020YFA0710203, 2023YFA1507400), the National Natural Science Foundation of China (22279146, 22102192, 22033009, 22293015 and 22121002), the CAS Project for Young Scientists in Basic Research (grant number YSBR-050) and the Photon Science Center for Carbon Neutrality, China Postdoctoral Science Foundation (BX20200336 and 2020M680680), S&T Program of Hebei (B2021208074).

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, People’s Republic of China

    Jiyuan Liu, Pengsong Li, Yong Wang, Lihong Jing, Zhimin Liu, Jianling Zhang, Qingli Qian, Xinchen Kang, Xiaofu Sun, Qinggong Zhu & Buxing Han

  2. School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, People’s Republic of China

    Jiyuan Liu, Pengsong Li, Yong Wang, Lihong Jing, Zhimin Liu, Jianling Zhang, Qingli Qian, Xinchen Kang, Xiaofu Sun, Qinggong Zhu & Buxing Han

  3. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, People’s Republic of China

    Shuaiqiang Jia & Buxing Han

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  1. Jiyuan Liu
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Contributions

Q.Z. and B.H. conceived and supervised the project. J.L., Q.Z. and B.H. wrote the paper. J.L. conducted the experimental work. P.L., S.J., Y.W., L.J., Z.L., J.Z., Q.Q., X.K. and X.S. assisted with X-ray diffraction, SEM, NMR, TEM and XAFS measurements. All authors discussed the results and contributed to the final paper.

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Correspondence to Qinggong Zhu or Buxing Han.

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Supplementary Methods, Notes 1–5, Figs. 1–80, Tables 1–7 and references 1–53.

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Liu, J., Li, P., Jia, S. et al. Electrocatalytic CO2 hydrogenation to C2+ alcohols catalysed by Pr–Cu oxide heterointerfaces. Nat. Synth 4, 730–743 (2025). https://doi.org/10.1038/s44160-025-00752-4

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