DOE OSTI · 3365377
Chirality-induced spin selectivity as a mechanism to control product selectivity during electrochemical CO 2 reduction
Abstract
Electrocatalytic CO 2 reduction often suffers from competition with the hydrogen evolution reaction (HER), which lowers efficiency and limits product selectivity. Recent studies suggest that electron spin, when controlled at an electrode surface, can influence reaction pathways, but direct evidence linking spin effects to suppressed HER has been limited. Here, in this work, we show that helical chiral copper (Cu) electrodes reduce competing HER during CO 2 reduction, consistent with spin polarization induced via the chiral-induced spin selectivity effect. The helically structured Cu electrodes are fabricated by electrodeposition with a chiral templating reagent. Time-resolved Kerr ellipticity measurements, which track spin-polarized carriers generated by an ultrafast Seebeck current, confirm spin accumulation at the chiral Cu surface. This spin polarization disfavours H—H bond formation, thereby suppressing HER and enabling formate production alongside CO. These findings demonstrate that chirality-based spin control offers a strategy for steering selectivity in CO 2 reduction and other reactions where HER is an undesired competitor.
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Tan, Jeiwan [National Laboratory of the Rockies (NLR), Golden, CO (United States); Korea Institute of Energy Technology (KENTECH) (Korea, Republic of)] (ORCID:0000000336276765), Shelton, Jacob L. [National Laboratory of the Rockies (NLR), Golden, CO (United States)] (ORCID:0000000278025545), Wright, Demelza [National Laboratory of the Rockies (NLR), Golden, CO (United States)], Haque, Md Azimul [National Laboratory of the Rockies (NLR), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)] (ORCID:0000000335280674), Saund, Simran S. [National Laboratory of the Rockies (NLR), Golden, CO (United States)], Ghoshal, Debjit [National Laboratory of the Rockies (NLR), Golden, CO (United States)], Le, Trung H. [National Laboratory of the Rockies (NLR), Golden, CO (United States)] (ORCID:0000000339138966), Dong, Yifan [National Laboratory of the Rockies (NLR), Golden, CO (United States)] (ORCID:0000000329123322), Smeaton, Michelle A. [National Laboratory of the Rockies (NLR), Golden, CO (United States)], Jungjohann, Katherine L. [National Laboratory of the Rockies (NLR), Golden, CO (United States)] (ORCID:0000000281321230), Miller, Elisa M. [National Laboratory of the Rockies (NLR), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)] (ORCID:0000000276485433), Beard, Matthew C. [National Laboratory of the Rockies (NLR), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)] (ORCID:0000000227111355), Neale, Nathan R. [National Laboratory of the Rockies (NLR), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)] (ORCID:0000000156541664), van de Lagemaat, Jao [National Laboratory of the Rockies (NLR), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)] (ORCID:0000000158516163). 2026-05-12. Chirality-induced spin selectivity as a mechanism to control product selectivity during electrochemical CO 2 reduction. https://doi.org/10.1038/s41560-026-02062-1
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