Maximizing the Formation of Reactive Oxygen Species for Deep Oxidation of NO via Manipulating the Oxygen-Vacancy Defect Position on (BiO)2CO3
Maximizing the Formation of Reactive Oxygen Species for Deep Oxidation of NO via Manipulating the Oxygen-Vacancy Defect Position on (BiO)2CO3
复制标题
通过操纵 (BiO)2CO3 上的氧空位缺陷位置最大限度地形成用于 NO 深度氧化的活性氧
DOI：
10.1021/acscatal.1c01251
复制
发表时间：
2021-06-11
期刊：
影响因子：
12.9
通讯作者：
Hojamberdiev, Mirabbos
中科院分区：
文献类型：
--
作者：
Rao, Fei;Zhu, Gangqiang;Hojamberdiev, Mirabbos
在金属氧化物半导体中构建氧空位（OVs）是一种有效而简单的方法，通过提高太阳光的利用率和促进表面活性氧（ROS）的形成来提高其光催化性能。在相同的晶体结构中存在不同的氧原子可能导致形成具有不同物理化学和光电性质的不同类型的OV。特别地，（BiO）（2）CO 3（BOC）的[BiO]（2）（2+）层中氧原子的两个不同晶体学位置允许构造两种类型的OV（OV 1和OV 2）。在本工作中，通过在BOC表面引入OVs 1和OVs 2，合成了OVs 1-BOC和OVs 2-BOC。通过分析光生载流子、吸附表面吸附物（H2O和O-2）的分离电位和氧化还原电位以及反应活化能，从理论和实验两方面研究了OVs 1和OVs 2对BOC中ROS生成的影响.通过可见光照射下的光氧化一氧化氮（NO）去除率来评价其光催化性能。OVsl-BOC和OVs 2-BOC表现出50.0和41.6%的光氧化NO去除效率，同时分别产生15.6和16.54ppb的NO2。原位傅里叶变换红外光谱和估算的NO转化途径揭示了OVs 1-BOC和OVs 2-BOC表面的光氧化NO去除机理和对NO2生成的抑制。这项工作展示了一种简单的方法，用于通过操纵半导体中的OV缺陷位置来增强光氧化NO去除。
Constructing oxygen vacancies (OVs) in metaloxide semiconductors is an effective and simple way to enhance the photocatalytic performance via promoting the utilization of solar light and boosting the formation of surface reactive oxygen species (ROS). The presence of different oxygen atoms in the same crystal structure can possibly lead to the formation of different types of OVs with distinct physicochemical and optoelectronic properties. Particularly, the two different crystallographic positions of oxygen atoms in the [BiO](2)(2+) layer of (BiO)(2)CO3 (BOC) allow the construction of two types of OVs (OVs1 and OVs2). In this work, OVs1-BOC and OVs2-BOC are synthesized via introducing the OVs1 and OVs2 on the surface of the BOC. The influence of OVs1 and OVs2 on the generation of ROS in the BOC is demonstrated based on theoretical and experimental studies by analyzing the separation and redox potentials of photogenerated charge carriers, absorption surface adsorbates (H2O and O-2), and reaction active energy. The photocatalytic performance is evaluated by photo-oxidative nitric oxide (NO) removal efficiency under visible light irradiation. The OVsl-BOC and OVs2-BOC exhibit 50.0 and 41.6% photo-oxidative NO removal efficiencies, while generating 15.6 and 16.54 ppb NO2, respectively. The in situ Fourier transform infrared spectroscopy and estimated NO conversion pathway reveal the photo-oxidative NO removal mechanism and suppression of NO2 formation on the surfaces of OVs1-BOC and OVs2-BOC. This work demonstrates a straightforward approach for enhancing the photo-oxidative NO removal via manipulating the OV defect position in semiconductors.