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pH-dependent KOW provides new insights in understanding the adsorption mechanism of ionizable organic chemicals on carbonaceous materials
Science of the Total Environment ( IF 9.8 ) Pub Date : 2017-11-10 , DOI: 10.1016/j.scitotenv.2017.11.065
Hao Li , Yanbei Cao , Di Zhang , Bo Pan

The dominant adsorption mechanism of ionizable organic chemicals (IOCs) on carbonaceous materials is still unclear. This study used benzoic acid (BA), o-chlorobenzoic acid (2-CBA) and p-chlorobenzoic acid (4-CBA) as representatives of IOCs to investigate the dominant adsorption mechanism on graphene oxide (GO) and graphite (GP), with a specific emphasis on the impact of pH-dependent KOW. The order of apparent adsorption of the investigated chemicals changed with pH, which could not be explained by their constant KOW. According to our measurement, KOW varied greatly with pH. The pH-dependent adsorption of BA, 2-CBA and 4-CBA were significantly correlated with pH-dependent KOW for both GO and GP. Our observations indicated that the hydrophobic effects may dominate the apparent adsorption of BA, 2-CBA and 4-CBA on GO and GP. Electrostatic repulsion played a minor role in their reduced adsorption at high pH. Negative charge-assisted H-bond and π-π interactions may explain the adsorption of negatively charged BA, 2-CBA and 4-CBA on negatively charged GO. This study implied that pH-dependent KOW rather than constant KOW should be incorporated to understand IOC adsorption as affected by pH.



中文翻译:

pH依赖性K OW为了解可电离有机化学物质在含碳材料上的吸附机理提供了新见识

含碳材料上可电离的有机化学物质(IOC)的主要吸附机理仍不清楚。本研究使用苯甲酸(BA),氯苯甲酸(2-CBA)和氯苯甲酸(4-CBA)作为IOC的代表,研究了氧化石墨烯(GO)和石墨(GP)的主要吸附机理,特别强调pH依赖性K OW的影响。所研究化学物质的表观吸附顺序随pH的变化而变化,这不能用其常数K OW来解释。根据我们的测量,K OW随pH值变化很大。对于GO和GP ,BA,2-CBA和4-CBA的pH依赖性吸附与pH依赖性K OW显着相关。我们的观察结果表明,疏水作用可能主导着BA,2-CBA和4-CBA在GO和GP上的表观吸附。静电排斥作用在高pH下降低吸附力方面起着次要作用。负电荷辅助的H键和π-π相互作用可以解释带负电荷的GO上带负电荷的BA,2-CBA和4-CBA的吸附。这项研究暗示应该结合pH依赖性的K OW而不是恒定的K OW来理解受pH影响的IOC吸附。

更新日期:2017-11-11
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