Ji Jiahui, Aleisa Rashed M, Duan Huan, Zhang Jinlong, Yin Yadong, Xing Mingyang
Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China.
Department of Chemistry, University of California, Riverside, Riverside, CA 92521, USA.
iScience. 2020 Feb 21;23(2):100861. doi: 10.1016/j.isci.2020.100861. Epub 2020 Jan 23.
Advanced oxidation processes (AOPs) based on sulfate radicals (SO) suffer from low conversion rate of Fe(III) to Fe(II) and produce a large amount of iron sludge as waste. Herein, we show that by using MoO as a cocatalyst, the rate of Fe(III)/Fe(II) cycling in PMS system accelerated significantly, with a reaction rate constant 50 times that of PMS/Fe(II) system. Our results showed outstanding removal efficiency (96%) of L-RhB in 10 min with extremely low concentration of Fe(II) (0.036 mM), outperforming most reported SO-based AOPs systems. Surface chemical analysis combined with density functional theory (DFT) calculation demonstrated that both Fe(III)/Fe(II) cycling and PMS activation occurred on the (110) crystal plane of MoO, whereas the exposed active sites of Mo(IV) on MoO surface were responsible for accelerating PMS activation. Considering its performance, and non-toxicity, using MoO as a cocatalyst is a promising technique for large-scale practical environmental remediation.
基于硫酸根自由基（SO）的高级氧化工艺（AOPs）存在Fe（III）向Fe（II）转化率低以及产生大量铁泥废弃物的问题。在此，我们表明通过使用MoO作为助催化剂，PMS体系中Fe（III）/Fe（II）循环速率显著加快，反应速率常数是PMS/Fe（II）体系的50倍。我们的结果显示，在极低浓度的Fe（II）（0.036 mM）下，10分钟内对L-RhB的去除效率高达96%，优于大多数已报道的基于SO的AOPs体系。表面化学分析结合密度泛函理论（DFT）计算表明，Fe（III）/Fe（II）循环和PMS活化均发生在MoO的（110）晶面上，而MoO表面暴露的Mo（IV）活性位点负责加速PMS活化。考虑到其性能和无毒特性，使用MoO作为助催化剂是一种有前景的大规模实际环境修复技术。
