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天然有机质在生物炭负载纳米镍铁降解十溴联苯醚过程中的影响作用机理辨识
  • ISSN号:0567-7351
  • 期刊名称:《化学学报》
  • 时间:0
  • 分类:TQ325.2[化学工程—合成树脂塑料工业]
  • 作者机构:[1]华南师范大学化学与环境学院,广州510006, [2]广东省水环境生态治理与修复工程技术研究中心,广州510006, [3]广东高校城市水环境生态治理与修复工程技术研宄中心,广州510006
  • 相关基金:项目受NSFC-广东联合基金(No.U1401235)资助.
中文摘要:

天然有机质(NOM)对纳米铁基材料去除污染物过程中的影响作用机理仍存争议.本工作选取腐殖酸(HA)作为NOM的代表物,研究了HA对生物炭负载纳米镍铁(BC@Ni/Fe)降解十溴联苯醚(BDE209)的动力学影响,结果表明HA对BC@Ni/Fe降解BDE209产生抑制作用,且随着HA浓度的升高,抑制作用越显著.通过HA与BC@Ni/Fe相互作用实验发现,HA能够快速地被BC@Ni/Fe吸附;通过HA对BC@Ni/Fe的Zeta电位和沉降影响实验发现,随着HA浓度的升高可有效提高BC@Ni/Fe的稳定性以及表面电荷,这表明HA不是通过影响BC@Ni/Fe颗粒的性能对BC@Ni/Fe去除BDE209产生抑制作用的.BC@Ni/Fe的腐蚀能力随着HA浓度的升高而降低,这与HA对BC@Ni/Fe去除BDE209反应活性影响成正相关关系.HA中具有电子传递作用的典型醌类化合物2-羟基-1,4-萘醌(Lawsone)和蒽醌-2,6-磺酸钠(AQDS),在反应过程中并没有起到电子传递作用促进反应进行,反而对BC@Ni/Fe去除BDE209起抑制作用.结合BDE209和HA之间的竞争吸附实验发现,HA抑制BC@Ni/Fe反应活性的主导原因是HA优先于BDE209被BC@Ni/Fe吸附,HA包覆于BC@Ni/Fe颗粒表面占据了活性位点,阻碍BC@Ni/Fe与H_2O的接触,减少了Fe^0的腐蚀,从而抑制了BC@Ni/Fe对BDE209的降解.

英文摘要:

The influence mechanism of natural organic matter (NOM) on the removal of contaminant by iron-based nanomaterials remains controversial. In this study, the effect of humic acid (representing NOM) on the degradation of decabromodiphenyl ether (BDE209) by biochar supported Ni/Fe nanoparticles (BC@Ni/Fe) were investigated, which indicated that the removal of BDE209 by BC@Ni/Fe was inhibited in the presence of HA, and with the increase of HA concentration, the inhibitory effect showed more significant. The interaction between HA and BC@Ni/Fe shown that HA was quickly adsorbed on the BC@Ni/Fe. The results of the Zeta potential and sedimentation experiment of BC@Ni/Fe showed that the stability and surface charge of BC@Ni/Fe were effectively improved with the increase of HA concentration, indicating that the inhibitory effect of HA in the debromination of BDE209 by BC@Ni/Fe was not through inhibiting the performance of nanoparticles by HA. The corrosion capacity of BC@Ni/Fe decreased with the increase of HA, which did positively correlate with the effect of HA on the reactivity of BC@Ni/Fe in the removal of BDE209. Additionally, those typical quinone compounds in HA (lawsone and AQDS), which have the electron transfer function, did not serve as an electron transfer medium to directly participating in the reaction process, on the contrary, those compounds did adversely effect on the removal of BDE209. In the coexisting system of HA and BDE209, the equilibrium adsorption capacity of HA on BC@Ni/Fe was 4.75 mg/g. Conversely, the adsorption quantities of BDE209 on BC@Ni/Fe in the absence of HA was 0.31 mg/g, which was about 1.3 times higher than that of in the presence of HA (the adsorption quantities of BDE209 was 0.23 mg/g). Moreover, in the coexistent system of HA and BDE209, the kinetic rate constants for the adsorption of HA was 0.1854 min-1, which was approximately 45 times greater than that of BDE209 (0.0041 min-1). It was shown from the analyzed results that the adsorption rate of HA on B

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期刊信息
  • 《化学学报》
  • 北大核心期刊(2014版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院上海有机化学研究所
  • 主编:周其林
  • 地址:上海市零陵路345号
  • 邮编:200032
  • 邮箱:hxxb@sioc.ac.cn
  • 电话:021-54925085
  • 国际标准刊号:ISSN:0567-7351
  • 国内统一刊号:ISSN:31-1320/O6
  • 邮发代号:4-209
  • 获奖情况:
  • 首届国家期刊奖,第二届国家期刊奖提名奖,中国期刊方阵“双高期刊”
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:28694