Exploring dopant effects in stannic oxide nanoparticles for CO2 electro-reduction to formate

Young-Jin Ko (), Jun-Yong Kim, Woong Hee Lee, Min Gyu Kim, Tae-Yeon Seong, Jongkil Park, YeonJoo Jeong, Byoung Koun Min, Wook-Seong Lee, Dong Ki Lee () and Hyung-Suk Oh ()
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Young-Jin Ko: Korea Institute of Science and Technology (KIST)
Jun-Yong Kim: Korea Institute of Science and Technology (KIST)
Woong Hee Lee: Korea Institute of Science and Technology (KIST)
Min Gyu Kim: Pohang Accelerator Laboratory (PAL)
Tae-Yeon Seong: Korea University
Jongkil Park: Korea Institute of Science and Technology (KIST)
YeonJoo Jeong: Korea Institute of Science and Technology (KIST)
Byoung Koun Min: Korea Institute of Science and Technology (KIST)
Wook-Seong Lee: Korea Institute of Science and Technology (KIST)
Dong Ki Lee: Korea Institute of Science and Technology (KIST)
Hyung-Suk Oh: Korea Institute of Science and Technology (KIST)

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract The electrosynthesis of formate from CO2 can mitigate environmental issues while providing an economically valuable product. Although stannic oxide is a good catalytic material for formate production, a metallic phase is formed under high reduction overpotentials, reducing its activity. Here, using a fluorine-doped tin oxide catalyst, a high Faradaic efficiency for formate (95% at 100 mA cm−2) and a maximum partial current density of 330 mA cm−2 (at 400 mA cm−2) is achieved for the electroreduction of CO2. Furthermore, the formate selectivity (≈90%) is nearly constant over 7 days of operation at a current density of 100 mA cm−2. In-situ/operando spectroscopies reveal that the fluorine dopant plays a critical role in maintaining the high oxidation state of Sn, leading to enhanced durability at high current densities. First-principle calculation also suggests that the fluorine-doped tin oxide surface could provide a thermodynamically stable environment to form HCOO* intermediate than tin oxide surface. These findings suggest a simple and efficient approach for designing active and durable electrocatalysts for the electrosynthesis of formate from CO2.

Date: 2022
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DOI: 10.1038/s41467-022-29783-7

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