<p>In situ observation of chemical reactions with high sensitivity and high spatiotemporal resolution is a long-standing goal in chemistry. Up to now, only a few, very specific systems can be studied. High-resolution operando imaging of chemical reactions typically requires a fluorescent probe to be included in the reaction. Here we introduce an operando microscopy methodology, namely quantum-sensing-enabled chemical operando microscopy (QCOM), in which reaction-induced local physical field changes are intrinsically transformed into dynamic imaging contrast using nitrogen vacancy centres in diamond. QCOM simultaneously satisfies the criteria of detection sensitivity (around four free radicals per pixel), spatial resolution (full-width-at-half-maximum resolution of around 312 nm) and temporal resolution (~10–240 ms). This has enabled the direct, quantitative, operando imaging of free-radical generation in the photocatalytic hydrolysis of TiO<sub>2</sub>, revealing an unexpected spatiotemporal sequential activation effect. Our work combines quantum sensing with chemical reaction imaging, offering a comprehensive in situ methodology to explore spatiotemporal phenomena in chemistry.</p><p></p>

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Quantum-sensing-enabled in situ imaging of free radicals in chemical reactions

  • Yibo Yang,
  • Zengrong Zhou,
  • Yang Xu,
  • Sijin Li,
  • Feihao Zhang,
  • Zihan Mao,
  • Chunxiao Zhao,
  • Wenjing Duan,
  • Shiyang Lyu,
  • Yunze Zhou,
  • Ziqing Zhang,
  • Wenxin Zhu,
  • Jiandong Feng

摘要

In situ observation of chemical reactions with high sensitivity and high spatiotemporal resolution is a long-standing goal in chemistry. Up to now, only a few, very specific systems can be studied. High-resolution operando imaging of chemical reactions typically requires a fluorescent probe to be included in the reaction. Here we introduce an operando microscopy methodology, namely quantum-sensing-enabled chemical operando microscopy (QCOM), in which reaction-induced local physical field changes are intrinsically transformed into dynamic imaging contrast using nitrogen vacancy centres in diamond. QCOM simultaneously satisfies the criteria of detection sensitivity (around four free radicals per pixel), spatial resolution (full-width-at-half-maximum resolution of around 312 nm) and temporal resolution (~10–240 ms). This has enabled the direct, quantitative, operando imaging of free-radical generation in the photocatalytic hydrolysis of TiO2, revealing an unexpected spatiotemporal sequential activation effect. Our work combines quantum sensing with chemical reaction imaging, offering a comprehensive in situ methodology to explore spatiotemporal phenomena in chemistry.