Reductive immobilization of radioactive pertechnetate(99TcO4^-) in simulated groundwater was studied by prepared carboxymethyl cellulose(CMC) and starch stabilized zero valent iron nanoparticles(nZVI),and long-term re...Reductive immobilization of radioactive pertechnetate(99TcO4^-) in simulated groundwater was studied by prepared carboxymethyl cellulose(CMC) and starch stabilized zero valent iron nanoparticles(nZVI),and long-term remobilization of reduced Tc was also evaluated under anoxic and oxic conditions.The stabilized nZVI can effectively reduce soluble 99Tc(Ⅶ) to insoluble 99 Tc(Ⅳ),and they can be easily delivered into a contaminated groundwater zone and facilitate in situ remediation.In this study,CMCstabilized nZVI showed higher reactivity than that using starch as the stabilizer.Batch experiments indicated that more than 99% of 99 Tc(Ⅶ)(CO=12 mg/mL) was reduced and removed from groundwater by CMC-stabilized nZVI with a CMC content of 0.2%(w/w) at a broad pH of 5-8.X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS) analyses further confirmed that 99Tc(Ⅶ)O4^-transformed into 99Tc(Ⅳ)O2(s).The presence of bicarbonate exhibited insignificant effect on Tc immobilization,while humic acid(HA) inhibited reaction mainly due to retardation on electron transfer and formation of Tc(IV)-HA complexes.More interesting,the immobilized Tc(Ⅳ) remained insoluble even after 120 d under anoxic condition,while only^21 % was remobilized when exposed to air.Therefore,biomacromolecules stabilized nZVI nanoparticles could be a viable alternative for in situ remediation of radioactive contamination in groundwater.展开更多
Technetium-99(~99Tc),largely produced by nuclear fission of ~235U or ~239Pu,is a component of radioactive waste.This study focused on a remediation strategy for the reduction of pertechnetate(Tc O_4^-)by studying its ...Technetium-99(~99Tc),largely produced by nuclear fission of ~235U or ~239Pu,is a component of radioactive waste.This study focused on a remediation strategy for the reduction of pertechnetate(Tc O_4^-)by studying its chemical analogue rhenium(Re(VⅡ))to avoid the complication of directly working with radioactive elements.Nanoscale zero-valent iron particles supported on graphene(NZVI/r GOs)from GOs-bound Fe ions were prepared by using a H_2/Ar plasma technique and were applied in the reductive immobilization of perrhenate(Re O_4^-).The experimental results demonstrated that NZVI/r GOs could efficiently remove Re from the aqueous solution,with enhanced reactivity,improved kinetics(50 min to reach equilibrium)and excellent removal capacity(85.77 mg/g).The results of X-ray photoelectron spectroscopy analysis showed that the mechanisms of Re immobilization by NZVI/r GOs included adsorption and reduction,which are significant to the prediction and estimation of the effectiveness of reductive Tc O_4^- by NZVI/r GOs in the natural environment.展开更多
基金partially supported by the National Natural Science Foundation of China(No.41230638)a grant from the USDA AAES 2015 Hatch and Multistate funding program
文摘Reductive immobilization of radioactive pertechnetate(99TcO4^-) in simulated groundwater was studied by prepared carboxymethyl cellulose(CMC) and starch stabilized zero valent iron nanoparticles(nZVI),and long-term remobilization of reduced Tc was also evaluated under anoxic and oxic conditions.The stabilized nZVI can effectively reduce soluble 99Tc(Ⅶ) to insoluble 99 Tc(Ⅳ),and they can be easily delivered into a contaminated groundwater zone and facilitate in situ remediation.In this study,CMCstabilized nZVI showed higher reactivity than that using starch as the stabilizer.Batch experiments indicated that more than 99% of 99 Tc(Ⅶ)(CO=12 mg/mL) was reduced and removed from groundwater by CMC-stabilized nZVI with a CMC content of 0.2%(w/w) at a broad pH of 5-8.X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS) analyses further confirmed that 99Tc(Ⅶ)O4^-transformed into 99Tc(Ⅳ)O2(s).The presence of bicarbonate exhibited insignificant effect on Tc immobilization,while humic acid(HA) inhibited reaction mainly due to retardation on electron transfer and formation of Tc(IV)-HA complexes.More interesting,the immobilized Tc(Ⅳ) remained insoluble even after 120 d under anoxic condition,while only^21 % was remobilized when exposed to air.Therefore,biomacromolecules stabilized nZVI nanoparticles could be a viable alternative for in situ remediation of radioactive contamination in groundwater.
基金the National Natural Science Foundation of China(21477133,41273134,91326202,21225730)
文摘Technetium-99(~99Tc),largely produced by nuclear fission of ~235U or ~239Pu,is a component of radioactive waste.This study focused on a remediation strategy for the reduction of pertechnetate(Tc O_4^-)by studying its chemical analogue rhenium(Re(VⅡ))to avoid the complication of directly working with radioactive elements.Nanoscale zero-valent iron particles supported on graphene(NZVI/r GOs)from GOs-bound Fe ions were prepared by using a H_2/Ar plasma technique and were applied in the reductive immobilization of perrhenate(Re O_4^-).The experimental results demonstrated that NZVI/r GOs could efficiently remove Re from the aqueous solution,with enhanced reactivity,improved kinetics(50 min to reach equilibrium)and excellent removal capacity(85.77 mg/g).The results of X-ray photoelectron spectroscopy analysis showed that the mechanisms of Re immobilization by NZVI/r GOs included adsorption and reduction,which are significant to the prediction and estimation of the effectiveness of reductive Tc O_4^- by NZVI/r GOs in the natural environment.