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<p>Harnessing sunlight, carbon dioxide, and water to produce two-carbon products is promising but constrained by sluggish kinetics and high carbon–carbon coupling barriers. Here, we report Ni single-atom anchored twisted SnS<sub>2</sub> (Ni-TSnS<sub>2</sub>) for ethane (C<sub>2</sub>H<sub>6</sub>) photosynthesis. In-situ electron paramagnetic resonance was developed to observe spin-orbit coupling in Ni-TSnS<sub>2</sub>. Spontaneous long-range spin-momentum locking originated from spin-orbit coupling enables magnetic-field-free long-range spin pinning. Topological protection inherent to long-range spin-momentum locking enhances its stability and ensures spin-polarized electron supply for charge separation. In-situ electron paramagnetic resonance further revealed single-electron transfer at Ni sites during CO<sub>2</sub> reduction. Single-electron transfer raised from spin-orbit coupling induces surface-adsorbed methyl intermediate to form methyl radicals (·CH<sub>3</sub>). ·CH<sub>3</sub>-to-C<sub>2</sub>H<sub>6</sub> chain reaction pathway enhances C<sub>2</sub>H<sub>6</sub> photosynthesis and selectivity. Consequently, Ni-TSnS<sub>2</sub> achieves a C<sub>2</sub>H<sub>6</sub> production rate of 139.58 ±  5.14 μmol g<sup>-1</sup> h<sup>-1</sup> with 89.41 ±  4.43% electron selectivity. In this work, we propose a twist engineering strategy to modulate spin states of charge, thereby promoting charge separation and single-electron transfer in photoreduction of CO<sub>2</sub> to C<sub>2</sub>H<sub>6</sub>.</p>

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Twist engineering induced spin-orbit coupling for photosynthesis of ethane from carbon dioxide and water

  • 期刊论文

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  • 发表日期：

    2026年1月30日

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  • Zhaoli Liu,
  • Yixuan Gao,
  • Long Chen,
  • Alistair G. L. Borthwick,
  • Weiliang Sun,
  • Peishen Li,
  • Wen Liu

摘要

Harnessing sunlight, carbon dioxide, and water to produce two-carbon products is promising but constrained by sluggish kinetics and high carbon–carbon coupling barriers. Here, we report Ni single-atom anchored twisted SnS2 (Ni-TSnS2) for ethane (C2H6) photosynthesis. In-situ electron paramagnetic resonance was developed to observe spin-orbit coupling in Ni-TSnS2. Spontaneous long-range spin-momentum locking originated from spin-orbit coupling enables magnetic-field-free long-range spin pinning. Topological protection inherent to long-range spin-momentum locking enhances its stability and ensures spin-polarized electron supply for charge separation. In-situ electron paramagnetic resonance further revealed single-electron transfer at Ni sites during CO2 reduction. Single-electron transfer raised from spin-orbit coupling induces surface-adsorbed methyl intermediate to form methyl radicals (·CH3). ·CH3-to-C2H6 chain reaction pathway enhances C2H6 photosynthesis and selectivity. Consequently, Ni-TSnS2 achieves a C2H6 production rate of 139.58 ±  5.14 μmol g-1 h-1 with 89.41 ±  4.43% electron selectivity. In this work, we propose a twist engineering strategy to modulate spin states of charge, thereby promoting charge separation and single-electron transfer in photoreduction of CO2 to C2H6.