Despite the significance of singlet oxygen (¹O₂) in several biological, chemical, and energy storage systems, its voltammetric reduction at an electrode remains unreported. We address this issue using nanogap scanning electrochemical microscopy (SECM) in substrate-generation/tip-collection mode. Our investigation reveals a reductive process on the SECM tip at −1.0 V (vs Fc⁺/Fc) during the breakdown of the Li₂CO₃ substrate in deuterated acetonitrile. Notably, this value is approximately 0.9 V more positive than the reduction potential of triplet oxygen (³O₂), consistent with thermodynamic estimates for the energy of the formation of ¹O₂. This finding holds significant implications for understanding the reaction mechanisms involving ¹O₂ in nonaqueous media.

中文翻译：

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通过纳米间隙扫描电化学显微镜实现单线态氧的伏安检测

^{尽管单线态氧 ( 1} O ₂ ) 在多种生物、化学和能量存储系统中具有重要意义，但其在电极上的伏安还原仍未有报道。我们使用纳米间隙扫描电化学显微镜（SECM）在基底生成/尖端收集模式下解决这个问题。我们的研究揭示了在氘代乙腈中Li ₂ CO ₃底物分解过程中SECM 尖端在 -1.0 V（相对于 Fc ⁺ /Fc）下的还原过程。值得注意的是，该值比三线态氧 ( ³ O _{2 ) 的还原电势高约 0.9 V，与}¹ O ₂形成能量的热力学估计一致。这一发现对于理解非水介质中涉及¹ O ₂的反应机制具有重要意义。