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<p>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<sub>1</sub>–ZnS<sub>v</sub>) that enables efficient and selective CO<sub>2</sub>-to-C<sub>2+</sub> 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-S<sub>2</sub> 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 Mn<sub>1</sub>–ZnS<sub>v</sub> catalyst achieved 99.1% selectivity for ethylene with a formation rate of 76.6 μmol g<sup>-1</sup> h<sup>-1</sup>. This study highlights the critical role of atomic-level coordination engineering in advancing photocatalytic CO<sub>2</sub>-to-C<sub>2+</sub> conversion.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月27日

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  • Zhiling Tang,
  • Yingli Wang,
  • Tian Qin,
  • Yuechang Wei,
  • Jing Xiong,
  • Xiong Wang,
  • Xuanzhen Li,
  • Min Liu,
  • Yunpeng Liu,
  • Xi Liu,
  • Zhen Zhao

摘要

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.