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

化学 催化作用 普鲁士蓝 反应速率常数 降级(电信) 路易斯酸 甲醇 核化学 多相催化 无机化学 动力学 有机化学 物理化学 物理 电信 量子力学 电化学 计算机科学 电极
作者
Hanxuan Zeng,Lin Deng,Lingfang Yang,Huiying Wu,Haojie Zhang,Chan Zhou,Bin Liu,Zhou Shi
出处
期刊:Chemical Engineering Journal [Elsevier]
卷期号:416: 128071-128071 被引量:52
标识
DOI:10.1016/j.cej.2020.128071
摘要

In this study, with two dimensional MXene as the substrate, Prussian blue [email protected] composite ([email protected]) 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−1 with 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−1 at 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 [email protected] 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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