Probing the Role of Atomic Defects in Photocatalytic Systems through Photoinduced Enhanced Raman Scattering
Probing the Role of Atomic Defects in Photocatalytic Systems through Photoinduced Enhanced Raman Scattering
复制标题
光诱导增强拉曼散射研究原子缺陷在光催化体系中的作用
DOI：
10.1021/acsenergylett.1c01772
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发表时间：
2021-11-11
影响因子：
22
通讯作者：
Cortes, Emiliano
中科院分区：
文献类型：
--
作者：
Glass, Daniel;Quesada-Cabrera, Raul;Cortes, Emiliano
即使在极少量的情况下，氧空位(VO)对金属氧化物半导体的电荷传输、表面吸附和反应性等关键性能也有很大的影响，在功能材料的性能中起着核心作用。目前用于研究VO的方法往往依赖于在远不理想的反应条件下使用专门的仪器。因此，催化过程中原位生成的VO的影响还有待于探讨。在这项工作中，我们现场评估了在光催化条件下非本征表面VO的形成和寿命，并与光催化性能进行了比较。我们首次证明了原位生成的原子VO的寿命在催化中的作用比它们的浓度更重要，并且较长的VO寿命与较高的光催化活性有很强的相关性。我们的结果表明，光催化效率的提高与金发姑娘的VO浓度有关，其中VO的浓度必须恰到好处，以鼓励载流子传输，同时避免电荷载流子捕获。
Even in ultralow quantities, oxygen vacancies (VO) drastically impact key properties of metal oxide semiconductors, such as charge transport, surface adsorption, and reactivity, playing central roles in functional materials performance. Current methods used to investigate VO often rely on specialized instrumentation under far from ideal reaction conditions. Hence, the influence of VO generated in situ during catalytic processes has yet to be probed. In this work, we assess in situ extrinsic surface VO formation and lifetime under photocatalytic conditions which we compare to photocatalytic performance. We show for the first time that lifetimes of in situ generated atomic VO play more significant roles in catalysis than their concentration, with strong correlations between longer-lived VO and higher photocatalytic activity. Our results indicate that enhanced photocatalytic efficiency correlates with goldilocks VO concentrations, where VO densities must be just right to encourage carrier transport while avoiding charge carrier trapping.