Novel Prussian blue analogues@MXene nanocomposite as heterogeneous activator of peroxymonosulfate for the degradation of coumarin: The nonnegligible role of Lewis-acid sites on MXene
Novel Prussian blue analogues@MXene nanocomposite as heterogeneous activator of peroxymonosulfate for the degradation of coumarin: The nonnegligible role of Lewis-acid sites on MXene
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新型普鲁士蓝类似物@MXene纳米复合材料作为过一硫酸盐的非均相活化剂用于香豆素的降解：MXene上路易斯酸位点的不可忽视的作用
DOI：
10.1016/j.cej.2020.128071
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发表时间：
2021-07
影响因子：
15.1
通讯作者：
Zhou Shi
中科院分区：
文献类型：
--
作者：
Hanxuan Zeng;Lin Deng;Lingfang Yang;Huiying Wu;Haojie Zhang;Chan Zhou;Bin Liu;Zhou Shi
本研究以二维MXene为底物，制备了普鲁士蓝类似物@MXene复合材料(PBA@MXene)，并基于过氧单硫酸盐活化将其用于香豆素(CuU)的非均相催化氧化降解。初始pH对降解过程影响较大，碱性pH比酸性pH更有利于CuU的降解。在pH3.0、5.0、6.6和10.0时，动力学速率常数分别为0.030、0.055、0.121和0.246×min-1。在pH为10.0时，反应时间为20min，TOC的去除效率为70.9%。自由基清除剂实验表明，在500nM叔丁醇存在下，随着溶液pH值从3.0增至10.0，反应速率常数从0.004逐渐增大到0.040−1，而加入500mM甲醇后，在−为3.05.0、6.610.0时，反应速率常数分别为0.002、0.001、0.002和0.002。机理研究表明，不同pH值下CuO降解的差异主要归因于催化剂表面不饱和的Ti-C-O(Lewis酸位)和末端的F-Ti。这项工作不仅证明了1.2PBA@MXene是一种有希望的PMS活化降解CuO的催化剂，而且清楚地阐明了MXene的Lewis酸位在MXene催化剂中的作用。
In this study, with two dimensional MXene as the substrate, Prussian blue analogues@MXene composite (PBA@MXene) was fabricated and utilized as a heterogeneous catalyst for the oxidative degradation of coumarin (COU) based on peroxymonosulfate activation. The initial pH strongly affected the degradation process, and the alkaline pH was beneficial to the COU degradation than the acidic pH. The kinetic rate constants were determined to be 0.030, 0.055, 0.121 and 0.246 min-1at pHs of 3.0, 5.0, 6.6 and 10.0, respectively. The TOC removal efficiency achieved at pH 10.0 was 70.9% in 20 min reaction time. Radical scavengers tests showed that in the presence of 500 mM tert-butyl alcohol (TBA), the rate constant was gradually enhanced from 0.004 to 0.040 min−1with increasing the solution pH from 3.0 to 10.0; while with the addition of 500 mM Methanol (Me), the rate constants were determined to be 0.002, 0.001, 0.002, and 0.002 min−1at pHs of 3.0, 5.0, 6.6, and 10.0, respectively. Mechanism study indicated that the differences in COU degradation at different pHs could be mainly ascribed to the unsaturated Ti-C-O (Lewis-acid site) and terminal F-Ti on the catalyst surface. This work not only demonstrated that 1.2PBA@MXene was a promisingly effective catalyst for PMS activation for COU degradation, but also clearly spelled out the role of Lewis-acid sites of MXene in MXene-based catalysts.
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影响因子：
16.6
作者：
Liang, Xiao;Garsuch, Arnd;Nazar, Linda F.
通讯作者：
Nazar, Linda F.
影响因子：
9.5
作者：
Vijayakumar, M.;Bhuvaneswari, M. S.;Hu, Jianzhi
通讯作者：
Hu, Jianzhi
DOI：
10.1016/j.scitotenv.2019.134539
发表时间：
2020-04
期刊：
The Science of the total environment
影响因子：
--
作者：
Cheng Luo;Rui Hou;Guanjun Chen;Chuangchuang Liu;Lihua Zhou;Yong Yuan
通讯作者：
Cheng Luo;Rui Hou;Guanjun Chen;Chuangchuang Liu;Lihua Zhou;Yong Yuan
影响因子：
15.1
作者：
Junjie You;Weiyi Sun;Shi-jun Su;Z. Ao;Chao Liu;Gang Yao;B. Lai
通讯作者：
Junjie You;Weiyi Sun;Shi-jun Su;Z. Ao;Chao Liu;Gang Yao;B. Lai
影响因子：
4.3
作者：
Born, SL;Api, AM;Hawkins, DR
通讯作者：
Hawkins, DR