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Ethylene electrosynthesis at low voltages enabled by dopant-induced modulation of the rate-determining step

Nature Synthesis volume 4, pages 1396–1407 (2025)Cite this article

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Abstract

CO2 electrolysis offers an attractive route for the sustainable production of ethylene. However, electrolysis in membrane electrode assembly (MEA) systems using conventional copper electrocatalysts is limited by low current densities and high operating voltages. Here we report a design strategy involving cobalt-based subsurface dopants to construct and stabilize catalytically active sites. In-depth experimental and theoretical investigations revealed that the dopants induce a shift in the rate-determining step for ethylene from CO* coupling to the chemical step: OCCO* + H* → OCCHO* + *. A Tafel slope of 54 mV per decade is observed, which is considerably lower than the value of 124 mV per decade seen for a reference copper catalyst. This enables MEA operation with a low full-cell voltage of 1.89 V at 0.5 A and stable operation for 145 h at 1 A. We showcase record MEA CO2-to-ethylene conversion at a current of 4 A, with a Faradaic efficiency of 70.6% and a full-cell energy efficiency of 25.2%. Techno-economic assessment indicates potential for profitability with a production cost close to the ethylene market price under optimistic conditions.

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Fig. 1: Schematic showing simplified proposed reaction pathways from CO2 to ethylene.
Fig. 2: Computational studies of PBA-derived copper sites, Cu(100) and Cu(111).
Fig. 3: Materials characterization and CO2R performance of PBA-derived catalysts.
Fig. 4: Cyclic voltammetry and spectroscopy studies of CoCu.
Fig. 5: Isotope studies of CoCu.
Fig. 6: MEA electrolyser system performance for CO2-to-C2H4.

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Data availability

The data supporting the findings of this study are available within the article and its Supplementary Information files. Should any raw data files be needed in another format, they are available from the corresponding author upon reasonable request. Source data are provided with this paper.

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Acknowledgements

We thank B. Johannessen and acknowledge the use of the Australian Synchrotron Facility at the Australian Nuclear Science and Technology Organisation (ANSTO) for collection of the in situ X-ray absorption spectroscopy (XAS) data used in this work. We also acknowledge the use of the X-ray Absorption Fine structure for catalysis (XAFCA) beamline of the Singapore Synchrotron Light Source (SSLS) for collection of the ex situ and in situ XAS data used in this work. In situ XAS, including X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS), was also performed in fluorescence mode in an in situ photocatalytic cell using a silicon drift detector at the BL32A beamline of TPS, National Synchrotron Radiation Research Center (NSRRC), Taiwan. We thank W. Nie and C. Hu for useful advice on Raman spectra analysis. Y.L. acknowledges support and funding from the A*STAR (Agency for Science, Technology and Research) under its LCER FI programme (award number U2102d2002) and an NRF Fellowship (award number NRF-NRFF14-2022-0003). This research is supported by the National Research Foundation, Prime Minister’s Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) programme (Development of Advanced Catalysts for Electrochemical Carbon Abatement, project code 370184872). The computational study is supported by the Marsden Fund Council from government funding (21-UOA-237) and Catalyst: Seeding General Grant (24-UOA-048-CSG), managed by Royal Society Te Apārangi. All DFT calculations were carried out on the New Zealand eScience Infrastructure (NeSI) high-performance computing facilities.

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  1. These authors contributed equally: Qin Yang, Xiu Wang, Jiguang Zhang.

Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, Republic of Singapore

    Qin Yang, Jiguang Zhang, Meng Wang, Bingqing Wang, Yipeng Zang & Yanwei Lum

  2. School of Chemical Sciences, The University of Auckland, Auckland, New Zealand

    Xiu Wang, Yu Mao & Ziyun Wang

  3. Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), Singapore, Republic of Singapore

    Jiguang Zhang, Surani Bin Dolmanan, Mingsheng Zhang & Yanwei Lum

  4. Institute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR), Singapore, Republic of Singapore

    Shibo Xi & Wan Ru Leow

  5. Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, Taiwan

    Yu-Chun Liu, Yung-Hsi Hsu & Sung-Fu Hung

  6. Yunnan Key Laboratory for Micro/Nano Materials & Technology, National Center for International Research on Photoelectric and Energy Materials, School of Materials and Energy, Yunnan University, Kunming, China

    Longzhou Zhang

  7. Centre for Hydrogen Innovations, National University of Singapore, Singapore, Republic of Singapore

    Yanwei Lum

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Contributions

Y.L. and Z.W. supervised the project. Y.L. and Q.Y. conceived the idea and designed the experiments. Q.Y. carried out the experimental work. X.W. and Y.M. performed the computational work. J.Z. carried out the isotope experiments and analysis. Y.Z., S.X., Y.-C.L., Y.-H.H. and S.-F.H. carried out the XAS experiments. L.Z. performed the high-resolution STEM. S.B.D. carried out the X-ray diffraction measurements. M.W. prepared the Cu/PTFE and Cu/CP catalysts. B.W. prepared the IrOx-coated titanium mesh electrodes. M.Z. carried out the XPS measurements. W.R.L. contributed to data analysis and manuscript editing. Q.Y., X.W., Z.W. and Y.L. co-wrote the manuscript. All authors discussed the results and assisted with the manuscript preparation.

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Correspondence to Ziyun Wang or Yanwei Lum.

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Competing interests

Q.Y. and Y.L. are co-inventors on a patent application ‘Method of converting carbon dioxide to a multi-carbon compound’, PCT/SG2024/050727. The other authors declare no competing interests.

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Nature Synthesis thanks William Goddard III, Jingshan Luo and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Peter Seavill, in collaboration with the Nature Synthesis team.

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Atomic coordinates of the optimized computational models.

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Yang, Q., Wang, X., Zhang, J. et al. Ethylene electrosynthesis at low voltages enabled by dopant-induced modulation of the rate-determining step. Nat. Synth 4, 1396–1407 (2025). https://doi.org/10.1038/s44160-025-00850-3

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