Ampere-level co-electrosynthesis of formate from CO2 reduction paired with formaldehyde dehydrogenation reactions

Zhengyuan Li, Peng Wang, Guanqun Han, Shize Yang, Soumyabrata Roy, Shuting Xiang, Juan D. Jimenez, Vamsi Krishna Reddy Kondapalli, Xiang Lyu, Jianlin Li, Alexey Serov, Ruizhi Li, Vesselin Shanov, Sanjaya D. Senanayake, Anatoly I. Frenkel, Pulickel M. Ajayan, Yujie Sun (), Thomas P. Senftle () and Jingjie Wu ()
Additional contact information
Zhengyuan Li: University of Cincinnati
Peng Wang: Rice University
Guanqun Han: University of Cincinnati
Shize Yang: Arizona State University
Soumyabrata Roy: Indian Institute of Technology Kanpur
Shuting Xiang: Stony Brook University
Juan D. Jimenez: Brookhaven National Laboratory
Vamsi Krishna Reddy Kondapalli: University of Cincinnati
Xiang Lyu: Oak Ridge National Laboratory
Jianlin Li: Argonne National Laboratory
Alexey Serov: Oak Ridge National Laboratory
Ruizhi Li: University of Cincinnati
Vesselin Shanov: University of Cincinnati
Sanjaya D. Senanayake: Brookhaven National Laboratory
Anatoly I. Frenkel: Stony Brook University
Pulickel M. Ajayan: Rice University
Yujie Sun: University of Cincinnati
Thomas P. Senftle: Rice University
Jingjie Wu: University of Cincinnati

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Current catalysts face challenges with low formate selectivity at high current densities during the CO2 electroreduction. Here, we showcase a versatile strategy to enhance the formate production on p-block metal-based catalysts by incorporating noble metal atoms on their surface, refining oxygen affinity, and tuning adsorption of the critical oxygen-bound *OCHO intermediate. The formate yield is observed to afford a volcano-like dependence on the *OCHO binding strength across a series of modified catalysts. The rhodium-dispersed indium oxide (Rh/In2O3) catalyst exhibits impressive performances, achieving Faradaic efficiencies (FEs) of formate exceeding 90% across a broad current density range of 0.20 to 1.21 A cm−2. In situ Raman spectroscopy and theoretical calculations reveal that the oxophilic Rh site facilitates *OCHO formation by optimizing its adsorption energy, placing Rh/In2O3 near the volcano-shaped apex. A bipolar electrosynthesis system, coupling the CO2 reduction at the cathode with the formaldehyde oxidative dehydrogenation at the anode, further boosts the FE of formate to nearly 190% with pure hydrogen generation under an ampere-level current density and a low cell voltage of 2.5 V in a membrane electrode assembly cell.

Date: 2025
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DOI: 10.1038/s41467-025-60008-9

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