纳米N-C/ZrO_(2)活化过硫酸盐降解苯酚的机理研究  

The mechanism on activation of peroxymonosulfate using nano N-C/ZrO_(2) for phenol degradation

作　　者：刘创创 王逸[1] 周丽华 江峰 袁勇 LIU Chuangchuang;WANG Yi;ZHOU Lihua;JIANG Feng;YUAN Yong(School of Environmental Science and Engineering,Guangdong University of Technology,Guangzhou 510006;School of Biomedical and Pharmaceutical Sciences,Guangdong University of Technology,Guangzhou 510006;Army Institute of Engineering Design,Nanjing 210000)

机构地区：[1]广东工业大学环境科学与工程学院,广州510006 [2]广东工业大学生物医药学院,广州510006 [3]陆军研究院工程设计研究所,南京210000

出　　处：《环境科学学报》2021年第10期3956-3968,共13页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.41907122,51678162,41877045,21876032)。

摘　　要：锆基纳米材料具有很好的物理化学稳定性及较高的比表面积,适用于解决传统过渡金属基催化剂活化过硫酸盐时金属浸出等问题.本研究将氯化锆-尿素络合物通过热解法合成了一种氮掺杂碳/氧化锆复合材料(N-C/ZrO_(2)),用于活化过硫酸盐降解水中苯酚,并采用SEM、XRD、XPS和FTIR技术对N-C/ZrO_(2)进行表征.结果表明,N-C/ZrO_(2)催化材料是直径小于50 nm的纳米颗粒,且氮掺杂量为3.6%~4.9%;在pH=6~7的硼酸缓冲体系中,N-C/ZrO_(2)催化过硫酸盐可在30 min内使水中苯酚(20 mg·L^(-1))的降解率达99%,且催化剂具有良好的化学稳定性和可重复利用性.淬灭和电子顺磁共振(EPR)结果表明,在N-C/ZrO_(2)/PMS体系中,苯酚的降解是以1O_(2)为主要氧化物质的非自由基氧化过程.本研究为Zr基纳米材料在活化过硫酸盐降解污染物领域的应用提供了理论基础.Zirconium-based nanomaterials with high physical and chemical stability and surface area,have emerged as catalyst for persulfate activation with less extraction than that of traditional transition metal catalyst.A nano nitride-doped carbon-zirconia(N-C/ZrO_(2))was fabricated via a facile thermal pyrolysis method using zirconium chloride(ZrCl4)and urea as a zirconia precursor and nitride-carbon source,respectively.The N-C/ZrO_(2) was used to catalyze persulfate activation for phenol degradation and its physicochemical properties were exanimated by Scanning electron microscope(SEM),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS)and Fourier transform infrared(FTIR).The result showed that the as-fabricated N-C/ZrO_(2) catalyst with 3.6%~4.9% N-doping and a particle size of<50 nm revealed an excellent catalytic capability with almost removal(99%)of 20 mg·L^(-1) phenol in 30 min in borate buffer solution(pH=6~7).Moreover,the N-C/ZrO_(2) catalyst exhibited good chemical stability after five successive degradation cycles.The singlet oxygen(1O_(2))as the dominant reactive species in phenol degradation was confirmed by electron paramagnetic resonance spectroscopy(EPR)and scavenger experiments.This study demonstrated that the N-doped Zr-based nanomaterials in activating persulfate can be considered as a promising technology for the removal of aqueous organic contaminant.

关 键 词：过一硫酸盐 二氧化锆 苯酚 单线态氧 

分 类 号：X703[环境科学与工程—环境工程]