Enhanced catalytic activity of templated-double perovskite with 3D network structure for salicylic acid degradation under microwave irradiation: Insight into the catalytic mechanism

Enhanced catalytic activity of templated-double perovskite with 3D network structure for salicylic acid degradation under microwave irradiation: Insight into the catalytic mechanism
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具有3D网络结构的模板化双钙钛矿在微波辐射下增强水杨酸降解的催化活性:洞察催化机制

DOI:
10.1016/j.cej.2019.02.174
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发表时间:
2019-07
影响因子:
15.1
通讯作者:
Zhang Xiaodong
Zhang Xiaodong
中科院分区:
工程技术1区
文献类型:
--
作者:
Wang Yin;Wang Yun;Yu Lan;Wang Jiayuan;Du Baobao;Zhang Xiaodong

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水杨酸(SA)由于其生理毒性和在环境中的拟持久性而被认为是优先污染物。本研究提出了一种微波诱导双模板钙钛矿催化降解水杨酸的新技术,并将其应用于水杨酸水溶液的处理。一系列LaCo_(1-x)Cu_xO_3@PMMA采用聚甲基丙烯酸甲酯(PMMA)模板法合成了(X= 0,0.3,0.5,0.7,1)具有三维多孔网络结构的钙钛矿型催化剂,并用扫描电镜(SEM)、N2吸附-脱附(BET)、傅立叶变换红外光谱(FTIR)、X射线衍射(XRD)、X射线光电子能谱(XPS)和微波网络分析。结果表明,PMMA模板剂的加入和Cu(x= 0.5)的取代有利于合成具有高催化活性的LaCo 0.5Cu0.5O3@PMMA,其具有独特的三维多孔网络结构、较小的粒径分布、较好的微波吸收性能和较高的Co 3+/Co2+和Oads/Olatt比值。SA的去除符合准一级动力学模型,其降解效率随MW强度、溶液pH值和催化剂投加量的增加先增大后减小,随SA初始浓度的增加而减小。LaCo0.5Cu0.5O3@PMMA催化剂在重复实验中表现出良好的循环性和稳定性。结果表明,该催化剂的催化活性主要来自活性物种和分子量热点效应,其中dotOH和hVb+自由基在催化过程中起主要作用,分子量热点效应对降解的贡献较小。因此,LaCo 0.5Cu0.5O3@PMMA/MW技术具有降解速度快、二次污染小等优点,为水杨酸的处理提供了一条潜在的途径
Salicylic acid (SA) is considered as a priority pollutant due to its physiological toxicity and pseudo-persistence in the environment. In this study, a new catalytic degradation technology using microwave (MW) induced templated-double perovskite was proposed and applied in the treatment of SA in aqueous solution. A series of LaCo 1-x Cu x O 3@ PMMA (X= 0, 0.3, 0.5, 0.7, 1) perovskite-type catalysts with three-dimensionally porous network structure were synthesized by polymethylmethacrylate (PMMA) templating method, and characterized by scanning electron microscopy (SEM), N 2 adsorption-desorption analysis (BET), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and microwave network analysis. The results showed that the addition of PMMA template and substitution with Cu (x= 0.5) were beneficial to the generation of LaCo 0.5 Cu 0.5 O 3@ PMMA with high catalytic activity, which possessed unique 3D porous network structure, smaller particle size distribution, better microwave absorbing performance and higher ratios of Co 3+/Co 2+ and O ads/O latt. The SA removal fit pseudo-first-order model, and its degradation efficiency increased firstly and then decreased with the increase of MW intensity, solution pH and catalyst dosage, while decreased as initial SA concentration increasing. The LaCo 0.5 Cu 0.5 O 3@ PMMA catalyst presented favorable recycling and stability in the repeated experiment. The excellent catalytic activity was attributed to both active species and MW “hot spots”, among which radical dotOH and h vb+ played main roles in the catalytic process, and MW “hot spots” effect had a small contribution to the degradation. Hence, LaCo 0.5 Cu 0.5 O 3@ PMMA/MW technology with rapid degradation and negligible secondary pollution provides a potential way for treating salicylic acid in water.
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