Exceptional Visible-Light Activities of TiO2-Coupled N-Doped Porous Perovskite LaFeO3 for 2,4-Dichlorophenol Decomposition and CO2 Conversion
Exceptional Visible-Light Activities of TiO2-Coupled N-Doped Porous Perovskite LaFeO3 for 2,4-Dichlorophenol Decomposition and CO2 Conversion
复制标题
TiO2 耦合 N 掺杂多孔钙钛矿 LaFeO3 对 2,4-二氯苯酚分解和 CO2 转化具有出色的可见光活性
DOI：
10.1021/acs.est.6b04958
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发表时间：
2016-12-20
影响因子：
11.4
通讯作者：
Jing, Liqiang
中科院分区：
文献类型：
--
作者：
Humayun, Muhammad;Qu, Yang;Jing, Liqiang
在这项工作中，通过湿化学工艺成功制备了TiO2耦合的N掺杂多孔钙钛矿型LaFeO3纳米复合材料作为高效、廉价、稳定的可见光光催化剂。结果表明，与由于表面积大而具有相当高光活性的多孔 LaFeO3 相比，经过用量优化的纳米复合材料表现出优异的可见光光催化活性，可通过类似于 3 倍的增强来降解 2,4-二氯苯酚 (2,4-DCP)，并通过类似于 4 倍的增强来将 CO2 转化为燃料。通过各种实验数据，特别是中心点OH量评估，清楚地表明，光活性的显着增强归因于引入孔隙增加的比表面积，通过掺杂N形成表面态来扩展可见光吸收，以及通过耦合TiO2促进电荷转移和分离。此外，自由基捕获实验证实光生空穴是光催化降解2,4-DCP的主要氧化剂。此外，提出了一种可能的 2,4-DCP 光催化降解机制，主要基于所得的关键中间体 2-氯琥珀酸，m/z = 153，它很容易转化为 CO2 和 H2O。这项工作为合成可见光响应的高活性钙钛矿型纳米光催化剂开辟了一条新的可行途径，用于有效的环境修复和能源生产。
In this work, TiO2-coupled N-doped porous perovskite-type LaFeO3 nanocomposites as highly efficient, cheap, stable, and visible-light photocatalysts have successfully been prepared via wet chemical processes. It is shown that the amount-optimized nanocomposite exhibits exceptional visible light photocatalytic activities for 2,4-dichlorophenol (2,4-DCP) degradation by similar to 3-time enhancement and for CO2 conversion to fuels by similar to 4-time enhancement, compared to the resulting porous LaFeO3 with rather high photoactivity due to its large surface area. It is clearly demonstrated, by means of various experimental data, especially for the center dot OH amount evaluation, that the obviously enhanced photoactivities are attributed to the increased specific surface area by introducing pores, to the extended visible-light absorption by doping N to create surface states, and to the promoted charge transfer and separation by coupling TiO2. Moreover, it is confirmed from radical trapping experiments that the photogenerated holes are the predominant oxidants in the photocatalytic degradation of 2,4-DCP. Furthermore, a possible photocatalytic degradation mechanism for 2,4-DCP is proposed mainly based on the resultant crucial intermediate, 2-chlorosuccinic acid with m/z = 153, that readily transform into CO2 and H2O. This work opens up a new feasible route to synthesize visible-light-responsive high-activity perovskite-type nanophotocatalysts for efficient environmental remediation and energy production.