Preparation of nano-Fe0 modified coal fly-ash composite and its application for U(VI) sequestration

Preparation of nano-Fe0 modified coal fly-ash composite and its application for U(VI) sequestration
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纳米Fe0改性粉煤灰复合材料的制备及其U(VI)封存应用

DOI:
10.1016/j.molliq.2018.05.118
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发表时间:
2018-09
影响因子:
6
通讯作者:
Xiangke Wang
Xiangke Wang
中科院分区:
化学2区
文献类型:
--
作者:
Zhongshan Chen;Jinlu Xing;Zengxin Pu;Xiangxue Wang;Shanye Yang;Benben Wei;Yuejie Ai;Xiang Li;Diyun Chen;Xiangke Wang

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以废弃的粉煤灰为原料,制备了纳米级零价铁(NZVI)修饰的CFA磁性复合材料(NZVI/CFA),并将其应用于水溶液中U(VI)离子的高效吸附。U(VI)离子在NZVI/CFA上的固定容量(0.6 2 mmol.g−1)大于裸露CFA(0.2 5 mmol.g−1)或NZVI(0.38 mmol.g−1)。U(VI)在NZVI和NZVI/CFA上的吸附在低pH时主要受外球表面络合控制,在高pH时主要受内球表面络合作用控制。热力学数据和吸附等温线分析表明,NZVI/CFA对U(VI)的吸附过程为自发吸热过程。主要的反应机理是,大部分可溶的U(VI)离子首先被吸附到NZVI/CFA上,然后在多孔的NZVI/CFA复合材料上被部分吸附的表面U(VI)还原为U(VI),这种协同作用影响了U(VI)从溶液中的去除。密度泛函计算结果表明,NZVI/CFA对U(VI)和U(IV)离子具有较强的吸附能力,且U(IV)物种的结合能大于U(VI)物种的结合能,表明NZVI/CFA对U(IV)的吸附能力高于U(VI)。结果表明,NZVI/CFA是一种适合于废水净化中大量实际出水中U(VI)的固定材料。
The nanoscale zero valent iron (NZVI) modified coal fly ash (CFA) magnetic composites (NZVI/CFA) were synthesized from the waste CFA and applied for the high-efficiency sequestration of U(VI) ions from water solution. The sequestration capacity of U(VI) ions on NZVI/CFA (0.62 mmol·g−1) was larger than that on bare CFA (0.25 mmol·g−1) or NZVI (0.38 mmol·g−1). The sequestration of U(VI) on NZVI and NZVI/CFA was primary controlled by outer-sphere surface complexation at low pH, and by inner-sphere surface complexation at high pH. According to the thermodynamic data and the adsorption isotherms' analysis, the U(VI) sorption process to the NZVI/CFA was spontaneous and endothermic. The main reaction mechanism was that, most of the soluble U(VI) ions were firstly adsorbed to NZVI/CFA and then the surface adsorbed U(VI) was partly reduced to U(VI) on the porous NZVI/CFA composites, and this synergistically affected U(VI) removal from solution to NZVI/CFA. The results of DFT calculation indicated that the NZVI/CFA had a strong sequestration capacity towards U(VI) and U(IV) ions, and the binding energy of U(IV) species was larger than that of U(VI) species, which evidenced the higher sorption of U(IV) than U(VI) on NZVI/CFA. The results showed that NZVI/CFA was an appropriate material for U(VI) sequestration from large volumes of actual effluent in wastewater cleanup.
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