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Immobilization of TBBPA on pyrogenic carbon subjected to natural organic matter under freeze–thawing conditions: insights into surface functionalization, coverage processes and binding affinity
Environmental Science: Nano ( IF 7.3 ) Pub Date : 2019/12/09 , DOI: 10.1039/c9en00819e
Jian Shen 1, 2, 3, 4 , Gordon Huang 1, 2, 3, 4 , Chunjiang An 4, 5, 6, 7 , Yao Yao 1, 2, 3, 4 , Xiaying Xin 4, 8, 9, 10 , Scott Rosendahl 4, 11, 12
Affiliation  

The long-term environmental effects of pyrogenic carbon have recently raised many concerns in terms of the fate and transport of emerging pollutants. This study explored the surface changes of geometric structure, functional groups, and site-energy distribution on pyrogenic carbon surfaces throughout a long-term physical aging process. Through synchrotron-based FTIR analysis, a homo-functionalization process was found to be the result of the consolidation of oxygen-containing groups with aromatic structures and the antagonization of other active hydroxyl groups in surface formation. Kinetic studies of TBBPA immobilization on pyrogenic carbon surfaces revealed a coverage process where TBBPA–humic acid, pyrogenic carbon–humic acid and pyrogenic carbon–TBBPA interactions can be formed. Isotherm analysis further indicated that the coverage process of natural organic matter (NOM) can enhance the processes of multilayer adsorption and thermodynamic alteration. Moreover, the results exhibited that site energies were dominated by O[double bond, length as m-dash]C–OH⋯O[double bond, length as m-dash]C–OH hydrogen bonds from NOM linkages, and O–H⋯O–H hydrogen bonds for TBBPA interactions were weakened by NOM coverage. Understanding such TBBPA interactions on carbonaceous porous materials will not only enrich the understanding of the transport of ionic pollutants under complex environmental conditions, but also support the evaluation of long-term environmental impacts of both naturally and artificially produced pyrogenic carbons.

中文翻译:

在冻融条件下将TBBPA固定在受天然有机物质作用的热解碳上:洞察表面功能化,覆盖过程和结合亲和力

热源碳的长期环境影响最近引起了新污染物的命运和运输方面的许多关注。这项研究探索了在长期物理老化过程中热解碳表面上几何结构,官能团和位能分布的表面变化。通过基于同步加速器的FTIR分析,发现均官能化过程是具有芳族结构的含氧基团的固结和表面形成中其他活性羟基的拮抗作用的结果。将TBBPA固定在热碳表面上的动力学研究表明,覆盖过程可形成TBBPA-腐殖酸,热碳-腐殖酸和热碳-TBBPA相互作用。等温线分析进一步表明,天然有机物(NOM)的覆盖过程可以增强多层吸附和热力学改变的过程。而且,结果表明位能主要由O决定。[双键,长度为m-破折号][双键,长度为m-破折号]NOM的连接会削弱C-OH⋯O C-OH氢键和用于TBBPA相互作用的O-H⋯O-H氢键。了解含碳多孔材料上的此类TBBPA相互作用不仅将丰富对复杂环境条件下离子污染物迁移的理解,而且还将支持评估天然和人工产生的热解碳的长期环境影响。
更新日期:2020-02-20
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