Operando Dual-Mode Spectro-Electro Tracking Reveals Oxygen-Driven Replenishment of Lattice Vacancies in Metal Oxides
作者：Xuewen Chen , Yanyan Lu , Haoming Bao , Yu Qiao , Shuai Zhang , Daoshuan Ding , Jincheng Ni , Huaiyuan Zhao , Jiamei Jin , Fei Xing , Qian Zhao , Hongwen Zhang , Weiping Cai
期刊：Chemical Engineering Journal
卷（期）页：
全文链接：www.sciencedirect.com/science/article/pii/S1385894726032948
This work introduces an operando dual-mode spectro-electro tracking strategy that synchronizes surface-enhanced Raman spectroscopy (SERS) with real-time electrical measurements, enabling simultaneous monitoring of surface chemical transformations, defect dynamics, and carrier transport. Applied to the O2-ZnO system, this approach reveals a reversible lattice‑oxygen-replenishment mechanism, directly linking surface defect chemistry to conductivity changes and providing quantitative insight into the kinetics of oxygen incorporation. Importantly, the oxygen-replenishment process requires sufficient thermal activation (100–200 °C) and is consistently observed across multiple oxides, including In2O3, SnO2, and Fe2O3, underscoring its universality. By capturing chemical and electronic processes concurrently, this platform enables precise determination of optimal oxygen partial pressure for formaldehyde oxidation and provides mechanistic insights beyond the reach of conventional single-mode techniques. Overall, this work establishes a general strategy for elucidating the dynamic coupling between surface chemistry and charge transport, offering a protentional framework for rational design and optimization of functional oxide materials.
期刊：Chemical Engineering Journal
卷（期）页：
全文链接：www.sciencedirect.com/science/article/pii/S1385894726032948
This work introduces an operando dual-mode spectro-electro tracking strategy that synchronizes surface-enhanced Raman spectroscopy (SERS) with real-time electrical measurements, enabling simultaneous monitoring of surface chemical transformations, defect dynamics, and carrier transport. Applied to the O2-ZnO system, this approach reveals a reversible lattice‑oxygen-replenishment mechanism, directly linking surface defect chemistry to conductivity changes and providing quantitative insight into the kinetics of oxygen incorporation. Importantly, the oxygen-replenishment process requires sufficient thermal activation (100–200 °C) and is consistently observed across multiple oxides, including In2O3, SnO2, and Fe2O3, underscoring its universality. By capturing chemical and electronic processes concurrently, this platform enables precise determination of optimal oxygen partial pressure for formaldehyde oxidation and provides mechanistic insights beyond the reach of conventional single-mode techniques. Overall, this work establishes a general strategy for elucidating the dynamic coupling between surface chemistry and charge transport, offering a protentional framework for rational design and optimization of functional oxide materials.
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