Nanostructured Co-Mn containing perovskites for degradation of pollutants: Insight into the activity and stability

Nanostructured Co-Mn containing perovskites for degradation of pollutants: Insight into the activity and stability
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含有钙钛矿的纳米结构钴锰用于污染物降解:深入了解活性和稳定性

DOI:
10.1016/j.jhazmat.2018.01.054
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发表时间:
2018
影响因子:
13.6
通讯作者:
Shao Zongping
Shao Zongping
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Miao Jie;Sunarso Jaka;Duan Xiaoguang;Zhou Wei;Wang Shaobin;Shao Zongping

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废水中持久性有机成分的高效氧化去除依赖于具有高催化活性、稳定性和可回收性的低成本多相催化剂。在这里,我们设计了一系列含有钙钛矿结构的纳米Co-Mn催化剂,LaCo1−xMnxO3+δ(LCm,x = 0,0.3,0.5,0.7和1.0),具有过化学计量比氧(δ > 0),通过活化过一硫酸盐(PMS)对多种持久性有机污染物的降解表现出优异的催化活性。对催化用液晶基团的性质进行了较为全面的研究。在LCM中,Co的催化活性与电子填充(Eg)之间存在“火山型”关系。其中,LaCo0.5Mn0.5O3+δ(LCM55)具有较好的催化活性,Eg= 1.27。LCM55较高的间隙氧离子扩散速率(DO2−= 1.58 ± 0.01 × 10−13cm2s−1)也是其催化活性的重要原因。LCM55稳定性的提高可归因于其较强的相对酸性(3.22)。此外,随着溶液pH的升高(pH ≥ 7),LCM55的有机降解速率加快,金属浸出率降低(0.004 mm),是一种潜在的环境修复材料。
The efficient oxidative removal of persistent organic components in wastewater relies on low-cost heterogeneous catalysts that offer high catalytic activity, stability, and recyclability. Here, we designed a series of nanostructured Co-Mn containing perovskite catalysts, LaCo1−xMnxO3+δ(LCM, x = 0, 0.3, 0.5, 0.7, and 1.0), with over-stoichiometric oxygen (δ > 0) to show superior catalytic activity for the degradation of a variety of persistent aqueous organic pollutants by activating peroxymonosulfate (PMS). The nature of LCM for catalysis was comprehensively investigated. A “volcano-shaped” correlation was observed between the catalytic activity and electron filling (eg) of Co in LCM. Among these compounds, LaCo0.5Mn0.5O3+δ(LCM55) exhibited an excellent activity with eg= 1.27. The high interstitial oxygen ion diffusion rate (DO2−= 1.58 ± 0.01 × 10−13cm2s−1) of LCM55 also contributes to its catalytic activity. The enhanced stability of LCM55 can be ascribed to its stronger relative acidity (3.22). Moreover, an increased solution pH (pH ≥ 7) generated a faster organic degradation rate and a decrease in metal leaching (0.004 mM) for LCM55 perovskite, justifying it as a potential material for environmental remediation.