Highly Efficient Utilization of Nano-Fe(0) Embedded in Mesoporous Carbon for Activation of Peroxydisulfate.
Highly Efficient Utilization of Nano-Fe(0) Embedded in Mesoporous Carbon for Activation of Peroxydisulfate.
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DOI：
10.1021/acs.est.9b02170
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发表时间：
2019-07
影响因子：
11.4
通讯作者：
Yunwen Wu;Xiaotong Chen;Yu Han;Dongting Yue;Xinde Cao;Yixin Zhao;X. Qian
中科院分区：
文献类型：
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作者：
Yunwen Wu;Xiaotong Chen;Yu Han;Dongting Yue;Xinde Cao;Yixin Zhao;X. Qian
纳米零价铁（nZVI）颗粒由于其独特的电子和化学性质，在环境科学和技术领域受到广泛关注。然而，纳米零价铁的聚集和氧化给环境修复的实际应用带来了很大的困难。本研究采用螯合辅助共组装和碳热还原的方法制备了纳米Fe（0）/介孔碳复合材料。纳米Fe（0）粒子表面包覆有石墨层，石墨层均匀分散在介孔碳骨架中。这种独特的结构使纳米Fe（0）粒子在空气中稳定存在20天以上。将其作为过硫酸盐（PDS）活化剂用于2，4，6-三氯苯酚（TCP）的氧化处理。MCFe对TCP的TOF值比FeSO 4和Fe 2 O3·FeO高近3倍，比商品nZVI高近2倍。MCFe活化PDS能有效地产生活性氧（ROS），包括·SO 4-、HO·和·O2-、1 O2。纳米Fe（0）粒子对PDS的活化过程是由固/水界面上连续产生的亚铁离子（Fe（II））诱导的。也就是说，纳米Fe（0）颗粒在基于硫酸根的高级氧化过程（SR-AOP）中被高效利用。多孔结构还有助于降解过程中TCP的吸收和转移。
Nano-scale zero valent iron (nZVI) particles have received much attention in environmental science and technology due to its unique electronic and chemical properties. However, the aggregation and oxidation of nZVI brings much difficulty in practical application of environmental remediation. In this study, we reported a composite nano-Fe(0)/mesoporous carbon by a chelation-assisted co-assembly and carbothermal reduction strategy. Nano-Fe(0) particles with surface iron oxide (Fe2O3·FeO) were wrapped with graphitic layers which were uniformly dispersed in mesoporous carbon frameworks. The unique structure made the nano-Fe(0) particles stable in air for more than 20 days. It was used as a peroxydisulfate (PDS) activator for the oxidation treatment of 2,4,6-trichlorophenol (TCP). The TOF value of MCFe for TCP degradation is nearly 3 times higher than those of FeSO4 and Fe2O3·FeO and nearly 2 times than that of commercial nZVI. The reactive oxygen species (ROS) including ·SO4-, HO· and ·O2-, 1O2 are efficiently generated by PDS activation with MCFe. The PDS activation process by nano-Fe(0) particles was intrinsically induced by the ferrous ions (Fe(II)) continuously generated at the solid/aqueous interface. Namely, the nano-Fe(0) particles were highly efficient utilized in sulfate radical-based advanced oxidation processes (SR-AOP). The porous structure also assists the absorption and transfer of TCP during the degradation process.