Similar to chromium contamination, the environmental contamination caused by uranium in radioactive coal bottom ash(CBA) is primarily dependent on the chemical speciation of uranium. However, the relationship betwee...Similar to chromium contamination, the environmental contamination caused by uranium in radioactive coal bottom ash(CBA) is primarily dependent on the chemical speciation of uranium. However, the relationship between uranium speciation and environmental contamination has not been adequately studied. To determine the relationship between uranium speciation and environmental contamination, X-ray absorption fine structure(XAFS) and X-ray photoelectron spectra(XPS) analyses were performed to determine the uranium speciation in CBA exposed to different chemical environments and simulated natural environments. The leachability of the different forms of uranium in the CBA was studied via a simulated acid rain leaching experiment, and the results showed that 57.0% of the total uranium was leached out as U(VI). The results of a linear combination fit(LCF)of the X-ray absorption near edge structure(XANES) spectrum revealed that in the raw CBA, the uranium mainly occurred as U_3O_8(71.8%). However, in the iron-rich particles, the uranium mainly occurred as UO_2(91.9%) after magnetic separation. Magnetite is a ubiquitous ferrousbearing oxide, and it was effective for the sorption of U(IV). The result of FeSO_4 leaching experiment indicated that 96.57% of total uranium was reduced from U(VI) to U(IV) when infiltrated with the FeSO_4 solution for 6 months. This result clearly demonstrated the changes in chemical valence of uranium in the coal ash and provided a conceptual principle for preventing uranium migration from ash to the surrounding soil and plants.展开更多
The radioactivity of uranium in radioactive coal bottom ash(CBA) may be a potential danger to the ambient environment and human health. Concerning the limited research on the distribution and mode of occurrence of u...The radioactivity of uranium in radioactive coal bottom ash(CBA) may be a potential danger to the ambient environment and human health. Concerning the limited research on the distribution and mode of occurrence of uranium in CBA, we herein report our investigations into this topic using a number of techniques including a five-step Tessier sequential extraction, hydrogen fluoride(HF) leaching, Siroquant(Rietveld) quantification, magnetic separation, and electron probe microanalysis(EPMA). The Tessier sequential extraction showed that the uranium in the residual and Fe–Mn oxide fractions was dominant(59.1%and 34.9%, respectively). The former was mainly incorporated into aluminosilicates,retained with glass and cristobalite, whereas the latter was especially enriched in the magnetic fraction, of which about 50% was present with magnetite(Fe_3O_4) and the rest in other iron oxides. In addition, the uranium in the magnetic fraction was 2.6 times that in the non-magnetic fraction. The experimental findings in this work may be important for establishing an effective strategy to reduce radioactivity from CBA for the protection of our local environment.展开更多
基金supported by the Talent Support Fund of Tsinghua University(No.413405001)
文摘Similar to chromium contamination, the environmental contamination caused by uranium in radioactive coal bottom ash(CBA) is primarily dependent on the chemical speciation of uranium. However, the relationship between uranium speciation and environmental contamination has not been adequately studied. To determine the relationship between uranium speciation and environmental contamination, X-ray absorption fine structure(XAFS) and X-ray photoelectron spectra(XPS) analyses were performed to determine the uranium speciation in CBA exposed to different chemical environments and simulated natural environments. The leachability of the different forms of uranium in the CBA was studied via a simulated acid rain leaching experiment, and the results showed that 57.0% of the total uranium was leached out as U(VI). The results of a linear combination fit(LCF)of the X-ray absorption near edge structure(XANES) spectrum revealed that in the raw CBA, the uranium mainly occurred as U_3O_8(71.8%). However, in the iron-rich particles, the uranium mainly occurred as UO_2(91.9%) after magnetic separation. Magnetite is a ubiquitous ferrousbearing oxide, and it was effective for the sorption of U(IV). The result of FeSO_4 leaching experiment indicated that 96.57% of total uranium was reduced from U(VI) to U(IV) when infiltrated with the FeSO_4 solution for 6 months. This result clearly demonstrated the changes in chemical valence of uranium in the coal ash and provided a conceptual principle for preventing uranium migration from ash to the surrounding soil and plants.
基金financial support from the Talent Support Fund of Tsinghua University (No. 413405001)
文摘The radioactivity of uranium in radioactive coal bottom ash(CBA) may be a potential danger to the ambient environment and human health. Concerning the limited research on the distribution and mode of occurrence of uranium in CBA, we herein report our investigations into this topic using a number of techniques including a five-step Tessier sequential extraction, hydrogen fluoride(HF) leaching, Siroquant(Rietveld) quantification, magnetic separation, and electron probe microanalysis(EPMA). The Tessier sequential extraction showed that the uranium in the residual and Fe–Mn oxide fractions was dominant(59.1%and 34.9%, respectively). The former was mainly incorporated into aluminosilicates,retained with glass and cristobalite, whereas the latter was especially enriched in the magnetic fraction, of which about 50% was present with magnetite(Fe_3O_4) and the rest in other iron oxides. In addition, the uranium in the magnetic fraction was 2.6 times that in the non-magnetic fraction. The experimental findings in this work may be important for establishing an effective strategy to reduce radioactivity from CBA for the protection of our local environment.