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具有丰富空位缺陷的MoS@MWCNTs通过内源性羟基自由基实现诺氟沙星的高效压电催化降解:增强非自由基途径及与自由基途径的协同机制

MoS@MWCNTs with Rich Vacancy Defects for Effective Piezocatalytic Degradation of Norfloxacin via Innergenerated-HO: Enhanced Nonradical Pathway and Synergistic Mechanism with Radical Pathway.

作者信息

Wang Xueyao, Hu Xuyang, Qu Zhengjun, Sun Ting, Huang Lihui, Xu Shimin

机构信息

School of Environmental Science and Engineering, Shandong University, No.72 Binhai Road, Jimo District, Qingdao, Shandong 266237, PR China.

Institute of Eco-Environmental Forensics, Shandong University, No.72 Binhai Road, Jimo District, Qingdao, Shandong 266237, PR China.

出版信息

ACS Appl Mater Interfaces. 2024 May 22;16(20):26257-26271. doi: 10.1021/acsami.4c04152. Epub 2024 May 10.

DOI:10.1021/acsami.4c04152
PMID:38728622
Abstract

Molybdenum disulfide (MoS)-based materials for piezocatalysis are unsatisfactory due to their low actual piezoelectric coefficient and poor electrical conductivity. Herein, 1T/3R phase MoS grown in situ on multiwalled carbon nanotubes (MWCNTs) was proposed. MoS@MWCNTs exhibited the interwoven morphology of thin nanoflowers and tubes, and the piezoelectric response of MoS@MWCNTs was 4.07 times higher than that of MoS via piezoresponse force microscopy (PFM) characterization. MoS@MWCNTs exhibited superior activity with a 91% degradation rate of norfloxacin (NOR) after actually working 24 min (as for rhodamine B, reached 100% within 18 min) by pulse-mode ultrasonic vibration-triggered piezocatalysis. It was found that piezocatalysis for removing pollutants was attributed to the synergistic effect of free radicals (OH and O) and nonfree radical (O, key role) pathways, together with the innergenerated-HO promoting the degradation rate. O can be generated by electron transfer and energy transfer pathways. The presence of oxygen vacancies (OVs) induced the transformation of O to O by triplet energy transfer. The fast charge transfer in MoS@MWCNTs heterostructure and the coexistence of sulfur vacancies and OVs enhanced charge carrier separation resulting in a prominent piezoelectric effect. This work opens up new avenues for the development of efficient piezocatalysts that can be utilized for environmental purification.

摘要

基于二硫化钼(MoS)的压电催化材料由于其实际压电系数低和导电性差而不尽人意。在此,提出了在多壁碳纳米管(MWCNTs)上原位生长的1T/3R相MoS。MoS@MWCNTs呈现出薄纳米花和纳米管的交织形态,通过压电响应力显微镜(PFM)表征,MoS@MWCNTs的压电响应比MoS高4.07倍。通过脉冲模式超声振动触发的压电催化,MoS@MWCNTs在实际工作24分钟后对诺氟沙星(NOR)表现出优异的活性,降解率为91%(对于罗丹明B,在18分钟内达到100%)。研究发现,去除污染物的压电催化归因于自由基(OH和O)和非自由基(O,起关键作用)途径的协同效应,以及内源性-HO促进降解率。O可以通过电子转移和能量转移途径产生。氧空位(OVs)的存在通过三重态能量转移诱导O向O的转变。MoS@MWCNTs异质结构中的快速电荷转移以及硫空位和OVs的共存增强了电荷载流子的分离,从而产生显著的压电效应。这项工作为开发可用于环境净化的高效压电催化剂开辟了新途径。

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