Utilization of renewable energies for catalytically generating value-added chemicals is highly desirable in this era of rising energy demands and climate change impacts. Artificial photosynthetic systems or photocatalysts utilize light to convert abundant CO₂, H₂O, and O₂ to fuels, such as carbohydrates and hydrogen, thus converting light energy to storable chemical resources. The emergence of intense X-ray pulses from synchrotrons, ultrafast X-ray pulses from X-ray free electron lasers, and table-top laser-driven sources over the past decades opens new frontiers in deciphering photoinduced catalytic reaction mechanisms on the multiple temporal and spatial scales. Operando X-ray spectroscopic methods offer a new set of electronic transitions in probing the oxidation states, coordinating geometry, and spin states of the metal catalytic center and photosensitizers with unprecedented energy and time resolution. Operando X-ray scattering methods enable previously elusive reaction steps to be characterized on different length scales and time scales. The methodological progress and their application examples collected in this review will offer a glimpse into the accomplishments and current state in deciphering reaction mechanisms for both natural and synthetic systems. Looking forward, there are still many challenges and opportunities at the frontier of catalytic research that will require further advancement of the characterization techniques.

中文翻译：

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使用 X 射线探针在多个时空尺度上破译自然和人工光合系统中的光诱导催化反应机制

在这个能源需求不断增长和气候变化影响的时代，利用可再生能源催化生产增值化学品是非常可取的。人工光合作用系统或光催化剂利用光将大量的CO ₂、H ₂ O和O ₂转化为燃料，例如碳水化合物和氢气，从而将光能转化为可储存的化学资源。过去几十年来，同步加速器产生的强 X 射线脉冲、X 射线自由电子激光器产生的超快 X 射线脉冲以及台式激光驱动源的出现，为破译多时空光诱导催化反应机制开辟了新的领域。空间尺度。Operando X 射线光谱方法提供了一组新的电子跃迁，以前所未有的能量和时间分辨率探测金属催化中心和光敏剂的氧化态、协调几何结构和自旋态。原位X 射线散射方法使得以前难以捉摸的反应步骤能够在不同的长度尺度和时间尺度上进行表征。本综述中收集的方法学进展及其应用实例将让我们了解在破译天然和合成系统的反应机制方面所取得的成就和现状。展望未来，催化研究前沿仍然存在许多挑战和机遇，需要进一步改进表征技术。