La-Doped ZnWO4 nanorods with enhanced photocatalytic activity for NO removal: effects of La doping and oxygen vacancies
La-Doped ZnWO4 nanorods with enhanced photocatalytic activity for NO removal: effects of La doping and oxygen vacancies
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具有增强光催化活性的 La 掺杂 ZnWO4 纳米棒去除 NO：La 掺杂和氧空位的影响
DOI：
10.1039/c9qi01152h
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发表时间：
2020-01
影响因子：
7
通讯作者：
Wang Qizhao
中科院分区：
文献类型：
--
作者：
Nie Junli;Qadeer-Ul Hassan;Jia Yuefa;Gao Jianzhi;Peng Jianhong;Lu Jiangbo;Zhang Fuchun;Zhu Gangqiang;Wang Qizhao
采用水热法制备了La 3+掺杂ZnWO 4纳米棒，并在模拟太阳光照射下对NO进行了光催化降解。光催化实验结果表明，掺镧量为0.6%的ZnWO 4纳米棒对NO的去除率最高，为46%。增强的光催化活性可以归因于La 3+离子掺杂，这产生了丰富的氧空位（OVs）的电子顺磁响应（EPR）证实。紫外-可见光谱结果表明，La 3+离子的掺杂和OVs的构建提高了材料的光学响应能力。密度泛函理论（DFT）计算结果表明，La 3+离子和高浓度OV的引入可以使ZnWO 4的禁带宽度变窄。通过清除剂实验和DMPO-ESR测量，发现e-和O2-自由基物种在氧化去除过程中发挥关键作用。此外，通过原位傅里叶变换红外光谱（in situ FTIR）对反应产物进行跟踪，提出了可能的光催化反应机理。总之，本工作的研究结果可以为设计和合成具有高效光催化NO去除的稀土离子掺杂和富OV光催化剂提供启发。
La3+-Doped ZnWO4 nanorods were prepared via a hydrothermal method for the photocatalytic NO removal under simulated solar light irradiation. It was revealed by photocatalytic experiments that the 0.6% La3+-doped ZnWO4 nanorods exhibited the best photocatalytic activities for NO removal (46%) in comparison with other samples. The enhanced photocatalytic activity could be attributed to La3+ ion doping, which creates an abundance of oxygen vacancies (OVs) as confirmed by the electron paramagnetic response (EPR). The optical response ability was promoted by La3+ ion doping and the construction of OVs according to the results of UV-vis spectra. Density functional theory (DFT) calculations were further conducted, revealing that the introduction of La3+ ions and high concentrations of OVs can narrow the band gap of ZnWO4. The e− and ˙O2− radical species are found to play critical roles in the oxidative removal process via the scavenger experiments and the DMPO-ESR measurements. Furthermore, the possible photocatalytic reaction mechanism was also proposed based on the products formed during the photocatalytic reaction, which were traced by in situ Fourier transform infrared spectroscopy (in situ FTIR). Overall, the findings in this work can provide inspiration for the design and synthesis of rare earth ion-doped and OV-rich photocatalysts with highly efficient photocatalytic NO removal.
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