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<p>Electrochemical O<sub>2</sub> activation offers a green approach for efficient synthesis of singlet oxygen (<sup>1</sup>O<sub>2</sub>). However, it is commonly determined by adsorption-dependent O<sub>2</sub> activation and transformation and can suffer from the sluggish desorption of surface-bound *OOH. Here we report an adsorption-independent O<sub>2</sub> activation pathway for <sup>1</sup>O<sub>2</sub> electrosynthesis via an O<sub>2</sub> mono-hydrogenation process on compressive-strained rutile TiO<sub>2</sub> (CSR-TiO<sub>2</sub>). This CSR-TiO<sub>2</sub> achieved an <sup>1</sup>O<sub>2</sub> generation rate of 148.26 μmol l<sup>−1</sup> min<sup>−1</sup> with near 100% Faradaic efficiency, outperforming the strain-free counterpart (35.97 μmol l<sup>−1</sup> min<sup>−1</sup>) and other previously reported materials. Such superior performance of CSR-TiO<sub>2</sub> stemmed from compressive strain, which can suppress the formation of reductive unsaturated sites for the O<sub>2</sub> adsorption and enhance the reductive ability of atomic hydrogen (H*), favouring the O<sub>2</sub> mono-hydrogenation pathway and bypassing the traditional surface-bound *OOH desorption pathway. The generated <sup>1</sup>O<sub>2</sub> could be utilized for the selective oxidation of thioanisole and its derivatives, offering a promising strategy for green organic synthesis.</p><p></p>

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Compressive-strained rutile TiO2 enables O2 mono-hydrogenation for singlet oxygen electrosynthesis

  • 期刊论文

  • 发表日期：

    2025年3月4日

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  • Ruizhao Wang,
  • Jie Dai,
  • Long Zhao,
  • Zhiwei Hu,
  • Chien-Te Chen,
  • Chang-Yang Kuo,
  • Guangming Zhan,
  • Yanbiao Shi,
  • Jiaxian Wang,
  • Yunjie Zou,
  • Mingkai Xu,
  • Xingyue Zou,
  • Qian Zheng,
  • Bing Zhou,
  • Kaiyuan Wang,
  • Rui Zhao,
  • Yan Zhang,
  • Yunhao Shen,
  • Yancai Yao,
  • Lizhi Zhang

摘要

Electrochemical O2 activation offers a green approach for efficient synthesis of singlet oxygen (1O2). However, it is commonly determined by adsorption-dependent O2 activation and transformation and can suffer from the sluggish desorption of surface-bound *OOH. Here we report an adsorption-independent O2 activation pathway for 1O2 electrosynthesis via an O2 mono-hydrogenation process on compressive-strained rutile TiO2 (CSR-TiO2). This CSR-TiO2 achieved an 1O2 generation rate of 148.26 μmol l−1 min−1 with near 100% Faradaic efficiency, outperforming the strain-free counterpart (35.97 μmol l−1 min−1) and other previously reported materials. Such superior performance of CSR-TiO2 stemmed from compressive strain, which can suppress the formation of reductive unsaturated sites for the O2 adsorption and enhance the reductive ability of atomic hydrogen (H*), favouring the O2 mono-hydrogenation pathway and bypassing the traditional surface-bound *OOH desorption pathway. The generated 1O2 could be utilized for the selective oxidation of thioanisole and its derivatives, offering a promising strategy for green organic synthesis.