Near-unity CO2-to-ethylene photoconversion over low coordination single-atom catalysts

Abstract 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 (Mn 1 –ZnS v ) that enables efficient and selective CO 2 -to-C 2+ 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…