Unlocking cathodic potential dependent Pd deactivation for energy efficient CO2 electroreduction to formate

Jingyi Chen, Mohammed Aliasgar, Yilin Zhao, Fernando Buendia Zamudio, Lei Fan, Junmei Chen, Jiayi Chen, Xiaosong Gu, Jiajia Gao, Sergey M. Kozlov () and Lei Wang ()
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Jingyi Chen: National University of Singapore, Department of Chemical and Biomolecular Engineering
Mohammed Aliasgar: National University of Singapore, Department of Chemical and Biomolecular Engineering
Yilin Zhao: National University of Singapore, Department of Chemical and Biomolecular Engineering
Fernando Buendia Zamudio: National University of Singapore, Department of Chemical and Biomolecular Engineering
Lei Fan: National University of Singapore, Department of Chemical and Biomolecular Engineering
Junmei Chen: National University of Singapore, Department of Chemical and Biomolecular Engineering
Jiayi Chen: National University of Singapore, Department of Chemical and Biomolecular Engineering
Xiaosong Gu: Southern University of Science and Technology, School of Environmental Science and Engineering
Jiajia Gao: Agency for Science, Technology and Research (A*STAR), Institute of Materials Research and Engineering (IMRE)
Sergey M. Kozlov: National University of Singapore, Department of Chemical and Biomolecular Engineering
Lei Wang: National University of Singapore, Department of Chemical and Biomolecular Engineering

Nature Communications, 2025, vol. 16, issue 1, 1-15

Abstract: Abstract Pd-based materials are among the best electrocatalysts with high CO2-to-formate selectivity at near-equilibrium potential. However, the efficiency of Pd is severely hindered by its deactivation at elevated overpotentials, resulting in limited formate production activity within a narrow potential window. Herein, by constructing a palladium/fullerene (PdC60) composite catalyst, we achieve improved activity towards formate production and enhanced resistance to deactivation at high overpotentials. As a result, the PdC60 composite achieves practically relevant current density of 250 mA cm−2 in 4 cm2 membrane electrode assembly reactor with a modest cell voltage of 1.71 V, along with the energy efficiency up to 72% towards formate, demonstrating its promise for future implementation. Mechanistically, we pinpoint the enhanced performance of PdC60 to the profound interfacial charge transfer from Pd to C60 substrate, which suppresses Pd-H phase transition and alleviates CO poisoning during catalysis. Overall, our discoveries shed light on the complex potential-dependent interplays between the phase evolution of Pd-based catalysts and CO2 electroreduction performance, highlighting its promise for energy-efficient CO2 conversion.

Date: 2025
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DOI: 10.1038/s41467-025-65255-4

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