Author
Listed:
- 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
Rice University)
- 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
University of Cincinnati)
- Sanjaya D. Senanayake
(Brookhaven National Laboratory)
- Anatoly I. Frenkel
(Stony Brook University
Brookhaven National Laboratory)
- Pulickel M. Ajayan
(Rice University)
- Yujie Sun
(University of Cincinnati)
- Thomas P. Senftle
(Rice University)
- Jingjie Wu
(University of Cincinnati)
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.
Suggested Citation
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 , 2025.
"Ampere-level co-electrosynthesis of formate from CO2 reduction paired with formaldehyde dehydrogenation reactions,"
Nature Communications, Nature, vol. 16(1), pages 1-9, December.
Handle:
RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-60008-9
DOI: 10.1038/s41467-025-60008-9
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