Photocatalytic conversion of carbon dioxide to value-added chemicals, particularly multi-carbon products, offers a promising route toward carbon-neutral cycles. However, achieving high activity and selectivity remains extremely challenging due to the instability of key reaction intermediates and limited C-C coupling efficiency. Herein, we report a low-coordination manganese single-atom catalyst embedded in zinc sulfide (Mn1-ZnSv) that enables efficient and selective CO2-to-C2+ conversion. In-situ spectroscopic analyses and density functional theory calculations reveal that sulfur vacancies are created at the Mn single-atom coordination sites and induce the formation of coordination-unsaturated Mn-S2 configuration. The asymmetric coordination environment of Mn modulates local charge distribution, strengthens *CO adsorption, and promotes *CO and *CHO coupling to form the *COCHO intermediate for efficient C-C coupling. As a result, the Mn1-ZnSv catalyst achieved 99.1% selectivity for ethylene with a formation rate of 76.6 μmol g-1 h-1. This study highlights the critical role of atomic-level coordination engineering in advancing photocatalytic CO2-to-C2+ conversion.
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Zhiling Tang
Yingli Wang
Tian Qin
Nature Communications
University of Chinese Academy of Sciences
Shanghai Jiao Tong University
Central South University
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Tang et al. (Tue,) studied this question.
www.synapsesocial.com/papers/69a75b91c6e9836116a23127 — DOI: https://doi.org/10.1038/s41467-026-68830-5