“碳中和”专刊系列文章（二十）｜天然电气石的多界面耦合实现抗生素高效去除：优越性与机理

Multiple interface coupling on natural tourmaline enables high-efficiency removal of antibiotic: Superior property and mechanism

Jingjing Cui, Xiangyu Liu, Feifan Qie, Chengzhe Xie, Qingdong He, Jian Liu^*, Steven L. Suib^*, Wenbo Wang^*

https://doi.org/10.1016/j.jes.2023.08.010

用于高效消除水中污染物的高活性、环境友好、高性价比催化剂的理性设计令人向往又充满挑战。我们制备了一种包含W/B/Fe协同活性中心的电气石氧化钨（TW10）高效多相光-芬顿催化剂。90%的廉价天然电气石矿石富含铁和硼元素。该催化剂可迅速活化过氧化单硫酸盐（PMS）产生大量活性自由基，从而引发四环素的快速高效降解。TW10/PMS/可见光体系在实际水样（包括海水、黄河水、长江水）中可有效降解高达97.8%的四环素，催化降解速率分别比电气石、氧化钨和商用P25高1.65、5.56和2.38倍。此外催化剂可循环多次使用。电子自旋共振谱、X射线光电子谱和液相质谱分析证实TW10催化剂上W/B/Fe 位点的协同催化效应加速了Fe(II)和Fe(III)以及W(V)和W(VI)之间的电子转移，从而促进了四环素的快速降解。我们探究了四环素的催化反应机理和降解路径。本工作为新型环境友好高效催化剂的设计和研发提供了一个可行的思路。

Reasonably designing highly active, environmentally friendly, and cost-effective catalysts for efficient elimination of pollutants from water is desirable but challenging. Herein, an efficient heterogeneous photo-Fenton catalyst tourmaline (TM)/tungsten oxide (WO3-x) (named TW10) containing tungsten/boron/iron (W/B/Fe) synergistic active centers and 90% of cheap natural tourmaline (TM) mineral rich in Fe and B elements. The TW10 catalyst can quickly activate peroxymonosulfate (PMS) to generate massive active free radicals, which may induce the rapid and efficient degradation of tetracycline (TC). The TW10/PMS/Visible light system can effectively degrade up to 98.7% of tetracycline (TC) in actual waters (i.e. seawater, Yellow River, and Yangtze River water), and the catalytic degradation rates reach 1.65, 5.569, and 2.38 times higher than those of TM, WO3-x, and commercial P25 (Degussa, Germany), respectively. In addition, the catalyst can be recycled and reused multiple times. Electron spin resonance spectroscopy (EPR), X-ray photoelectron spectroscopy (XPS), and liquid chromatograph-mass spectrometer (LC-MS) analyses confirm that the synergistic catalytic effect of W/B/Fe sites on the TW10 catalyst accelerates the electron transfer between Fe(II) and Fe(III), as well as between W(V) and W(VI), and thus promotes the rapid degradation of TC. The catalytic reaction mechanism and degradation pathway of TC were explored. This work provides a feasible route for the design and development of new eco-friendly and efficient catalyst.

通讯作者

刘健，内蒙古大学化学化工学院教授、院长、博导，教育部“长江学者奖励计划”特聘教授。长期致力于纳米多孔材料的设计合成及在能源、催化相关领域的基础应用研究。发表SCI学术论文170余篇，引用23000余次（H指数71）。曾获第14届国际催化大会青年科学家奖、国际先进材料学会奖章。

王文波，内蒙古大学化学化工学院教授，博士生导师。研究领域为（1）矿物功能材料的设计、构筑及应用；（2）天然生物质、固废资源清洁转化与高值利用；（3）原子经济性绿色可控合成与低碳生产新技术；（4）稀贵金属提取与分离。主持内蒙古自治区杰出青年科学基金项目等多个项目。共发表SCI论文180余篇，年度Top 1% ESI高被引论文3篇。论文总被引用6000余次，H指数43，入选全球前2%顶尖科学家榜单（位列前1%）。

https://www.sciencedirect.com/science/article/abs/pii/S1001074223003613

Jingjing Cui, Xiangyu Liu, Feifan Qie, Chengzhe Xie, Qingdong He, Jian Liu, Steven L. Suib, Wenbo Wang, 2024. Multiple interface coupling on natural tourmaline enables high-efficiency removal of antibiotic: Superior property and mechanism. J. Environ. Sci. 140, 242-254.