Reactant activation and photocatalysis mechanisms on Bi-metal@Bi2GeO5 with oxygen vacancies: A combined experimental and theoretical investigation
Reactant activation and photocatalysis mechanisms on Bi-metal@Bi2GeO5 with oxygen vacancies: A combined experimental and theoretical investigation
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氧空位 Bi-metal@Bi2GeO5 的反应物活化和光催化机制：实验与理论相结合的研究
DOI：
10.1016/j.cej.2019.04.003
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发表时间：
2019-08
影响因子：
15.1
通讯作者：
Fan Dong
中科院分区：
文献类型：
--
作者：
Xinwei Li;Wendong Zhang;Wen Cui;Jieyuan Li;Yanjuan Sun;Guangming Jiang;Hongwei Huang;Yuxin Zhang;Fan Dong
光催化过程遵循两个基本顺序：反应物吸附和表面光催化。在这项工作中，制备了Bi金属沉积的Bi2GeO5（Bi@BiGeO）作为模型光催化剂，以了解反应物的吸附和活化机制以及可见光照射下NO的光催化氧化。采用密度泛函理论和分析方法来揭示电子结构和光致载流子转移过程。 Bi金属的引入和BiGeO中氧空位（OV）的产生是通过一种简便的方法同时实现的。 Bi金属充当可见光天线和电子接收器，促进载流子分离和转移。 OV 促进反应物（H2O 和 O2）活化，从而增强活性氧 (ROS) 的产生。 NO分子被主动吸附在Bi@BiGeO上的配位不饱和位点上，并通过电子交换被激活。基于使用原位 FTIR 监测的反应中间体和最终产物，揭示了 Bi@BiGeO 上光催化 NO 氧化机理。这项工作强调了反应物活化作为设计高效光催化剂以克服环境应用瓶颈的新策略的重要性。
The photocatalysis process follows two fundamental sequences: reactant adsorption and surface photocatalysis. In this work, Bi metal-deposited Bi2GeO5(Bi@BiGeO) is prepared as a model photocatalyst to understand the adsorption and activation mechanisms of the reactants and the photocatalytic oxidation of NO under visible light irradiation. Density functional theory and analytical approaches are employed to reveal the electronic structure and photo-induced carrier transfer processes. The introduction of Bi metal and the generation of oxygen vacancies (OVs) in BiGeO were achieved simultaneously via a facile method. The Bi metal served as a visible light antenna and as an electron sink and promoted the carrier separation and transfer. The OVs promote reactant (H2O and O2) activation, thereby reinforcing the generation of reactive oxygen species (ROS). The NO molecules are actively adsorbed at the coordinative unsaturated sites on Bi@BiGeO and get activated via electron exchange. The photocatalytic NO oxidation mechanism on Bi@BiGeO is revealed based on the reaction intermediates and final products monitored using in-situ FTIR. This work highlights the importance of reactant activation as a new strategy for the design of highly efficient photocatalysts to overcome the bottlenecks in environmental applications.
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