研究报告

  • 刘创创,王逸,周丽华,江峰,袁勇.纳米N-C/ZrO2活化过硫酸盐降解苯酚的机理研究[J].环境科学学报,2021,41(10):3956-3968

  • 纳米N-C/ZrO2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/ZrO2 for phenol degradation
  • 基金项目:国家自然科学基金(No.41907122,51678162,41877045,21876032)
  • 作者
  • 单位
  • 刘创创
  • 广东工业大学环境科学与工程学院, 广州 510006
  • 王逸
  • 广东工业大学环境科学与工程学院, 广州 510006
  • 周丽华
  • 广东工业大学生物医药学院, 广州 510006
  • 江峰
  • 陆军研究院工程设计研究所, 南京 210000
  • 袁勇
  • 广东工业大学环境科学与工程学院, 广州 510006
  • 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/ZrO2),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/ZrO2进行表征.结果表明,N-C/ZrO2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/ZrO2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/ZrO2/PMS体系中,苯酚的降解是以1O2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.
  • Abstract: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/ZrO2) 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/ZrO2 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/ZrO2 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/ZrO2 catalyst exhibited good chemical stability after five successive degradation cycles. The singlet oxygen (1O2) 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.

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