Ordered Mesoporous Cobalt Containing Perovskite as a High-Performance Heterogeneous Catalyst in Activation of Peroxymonosulfate
Ordered Mesoporous Cobalt Containing Perovskite as a High-Performance Heterogeneous Catalyst in Activation of Peroxymonosulfate
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含钴有序介孔钙钛矿作为高性能多相催化剂用于过一硫酸盐的活化
DOI：
10.1021/acsami.9b11322
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发表时间：
2019
影响因子：
9.5
通讯作者：
Liang Heng
中科院分区：
文献类型：
--
作者：
Luo Xinsheng;Bai Langming;Xing Jiajian;Zhu Xuewu;Xu Daliang;Xie Binghan;Gan Zhendong;Li Guibai;Liang Heng
首次使用蒸发诱导自组装的简便方法合成了有序介孔钙钛矿 La2CoMnO6−δ(MLCMO)。 N2吸附、扫描电子显微镜和透射电子显微镜测量表明，优化的MLCMO具有高比表面积（58.7 m2/g）和均匀介孔（11.6 nm）。 MLCMO 在过一硫酸盐 (PMS) 活化和莠去津 (ATZ) 降解中表现出优异的催化性能。从比较来看，介孔 MLCMO 的催化活性优于块体 La2CoMnO6−δ(LCMO) 和其他常见的 PMS 活化剂，包括 α-MnO2、Co3O4 和 CoFe2O4。通过X射线光电子能谱、电子自旋共振和猝灭测试研究了MLCMO激活PMS的机制。 SO4•–、•OH、1O2 和O2•– 被确定为PMS 激活产生的主要活性氧。 MLCMO 中的 Co 和 Mn 是负责产生活性自由基的活性位点。参与 MnIII/MnIV 循环电子转移的晶格氧可逆氧化还原位点 (OL–/OL2–) 被证明是阳离子活性位点的氧化还原伙伴。此外，pH 11时SO4•–/•OH自由基转化得到促进，加速了PMS的消耗，严重抑制了ATZ的降解。
An ordered mesoporous perovskite, La2CoMnO6−δ(MLCMO), was synthesized for the first time using a facile method of evaporation-induced self-assembly. The N2-sorption, scanning electron microscopy, and transmission electron microscopy measurements indicated that the optimized MLCMO possessed a high specific surface area (58.7 m2/g) and was uniformly mesoporous (11.6 nm). The MLCMO exhibited superior catalytic performance in peroxymonosulfate (PMS) activation for atrazine (ATZ) degradation. From a comparison view, the catalytic activity of the mesoporous MLCMO outperformed that of the bulk La2CoMnO6−δ(LCMO) and other common PMS activators, including α-MnO2, Co3O4, and CoFe2O4. The mechanisms of PMS activation by the MLCMO were investigated by X-ray photoelectron spectroscopy, electron spin resonance, and quenching tests. SO4•–,•OH,1O2, and O2•–were identified as main reactive oxygen species generated from PMS activation. The Co and Mn in MLCMO were the active sites responsible for active radical generation. The lattice oxygen reversible redox sites (OL–/OL2–), which were involved in the electron transfer of the MnIII/MnIVcycle, were demonstrated as redox partners to the cation active sites. In addition, the SO4•–/•OH radical conversion was promoted at pH 11, which accelerated the consumption of PMS and seriously inhibited the degradation of ATZ.