DOI: 10.1002/anie.1640517 ISSN: 1433-7851

Spin Polarized Chiral Co 3 O 4 Boosts High‐Pressure CO 2 Electroreduction to Ethanol With 90% Sel

Mingliang Hu, Mingzi Sun, Runyao Zhao, Junjun Li, Yike Ye, Yu Zhang, Jiaju Fu, Bing Tang, Can Yu, Yunzhe Ke, Shuaishuai Ding, Bing Ni, Bo Wang, Chao Jin, Ruquan Ye, Zhimin Liu, Zhichuan J. Xu, Bolong Huang, Zhicheng Zhang, Wenping Hu

ABSTRACT

Electrocatalytic CO 2 reduction (CO 2 RR) to value‐added multicarbon products using non‐copper‐based catalysts remains a major challenge, especially for selective ethanol production. Herein, we report that chiral Co 3 O 4 featuring strong electron spin polarization achieves a maximum ethanol Faradaic efficiency of 90% at ‐0.9 V versus NHE in KHCO 3 electrolytes under a 30 bar CO 2 pressure, substantially outperforming both racemic Co 3 O 4 and previously reported non‐copper‐based catalysts. The enhanced spin polarization in chiral Co 3 O 4 facilitates electron transfer and promotes the activation of the adsorbed CO 2 , while also lowering the free energy change for C–C coupling to form *COCHO intermediate, thereby promoting ethanol production. Our work establishes spin polarization as a key determinant for efficient C–C coupling on non‐copper‐based catalysts and provides mechanistic principles for the rational design of CO 2 RR electrocatalyst.

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