Axial gas-liquid separators have been adopted in fission gas removal systems for the development of thorium molten salt reactors. In our previous study, we observed an unsteady flow phenomenon in which the flow patter...Axial gas-liquid separators have been adopted in fission gas removal systems for the development of thorium molten salt reactors. In our previous study, we observed an unsteady flow phenomenon in which the flow pattern is directly dependent on the backpressure in a gas-liquid separator; however, the underlying flow mechanism is still unknown. In order to move a step further in clarifying how the flow pattern evolves with a variation in backpressure, a large eddy simulation(LES) was adopted to study the flow field evolution. In the simulation, an artificial boundary was applied at the separator outlet under the assumption that the backpressure increases linearly. The numerical results indicate that the unsteady flow feature is captured by the LES approach, and the flow transition is mainly due to the axial velocity profile redistribution induced by the backpressure variation. With the increase in backpressure,the axial velocity near the downstream orifice transits from negative to positive. This change in the axial velocity sign forces the unstable spiral vortex to become a stable rectilinear vortex.展开更多
This work presents the results of computer simulation of neutronic processes in a high-temperature gas-cooled thorium reactor for 30 different options of core loading.To guarantee stable and long-term reactor operatio...This work presents the results of computer simulation of neutronic processes in a high-temperature gas-cooled thorium reactor for 30 different options of core loading.To guarantee stable and long-term reactor operation(7-10 years),the quantity of fuel compact dispersion phase and starting fuel composition was selected.It is demonstrated that it is possible in principle to substitute the near-axial recirculation zone of the reactor core by a long magnetic trap with a high-temperature plasma column for generating thermonuclear neutrons.The distribution of neutron yield along the length of the plasma source is also presented.Such a thorium reactor,with a near-axial source of extra neutrons,can be applied for researching thermophysical and neutronic characteristics of dispersion thorium fuel to improve its properties.The results of the work are of great interest from the perspective of future advancement of the thermonuclear power industry,by means of creation of a hybrid installation based on a thorium reactor with a long plasma column as a source of additional neutrons.展开更多
Herein, we assess the129I transmutation capability of a 2250-MWt single-fluid double-zone thorium molten salt reactor(SD-TMSR) by considering two methods. One is realized by loading an appropriate amount of129I before...Herein, we assess the129I transmutation capability of a 2250-MWt single-fluid double-zone thorium molten salt reactor(SD-TMSR) by considering two methods. One is realized by loading an appropriate amount of129I before the startup of the reactor, and the amount of129I during operation is kept constant by online feeding129I.The other adopts only an initial loading of129I before startup, and no other129I is fed online during operation.The investigation first focuses on the effect of the loading of I on the Th-233U isobreeding performance. The results indicate that a233U isobreeding mode can be achieved for both scenarios for a 60-year operation when the initial molar proportion of LiI is maintained within 0.40% and 0.87%, respectively. Then, the transmutation performances for the two scenarios are compared by changing the amount of injected iodine into the core. It is found that the scenario that adopts an initial loading of129I shows a slightly better transmutation performance in comparison with the scenario that adopts online feeding of129I when the net233U productions for the two scenarios are kept equal. The initial loading of129I scenario with LiI = 0.87% molar proportion is recommended for129I transmutation in the SD-TMSR,and can transmute 1.88 t of129I in the233U isobreeding mode over 60 years.展开更多
The high pressure behaviors of Th_4H_(15) and ThH_2 are investigated by using the first-principles calculations based on the density functional theory(DFT). From the energy–volume relations, the bct phase of ThH_...The high pressure behaviors of Th_4H_(15) and ThH_2 are investigated by using the first-principles calculations based on the density functional theory(DFT). From the energy–volume relations, the bct phase of ThH_2 is more stable than the fcc phase at ambient conditions. At high pressure, the bct ThH_2 and bcc Th_4H(15) phases are more brittle than they are at ambient pressure from the calculated elastic constants and the Poisson ratio. The thermodynamic stability of the bct phase ThH_2 is determined from the calculated phonon dispersion. In the pressure domain of interest, the phonon dispersions of bcc Th_4H(15) and bct ThH_2 are positive, indicating the dynamical stability of these two phases, while the fcc ThH_2 is unstable. The thermodynamic properties including the lattice vibration energy, entropy, and specific heat are predicted for these stable phases. The vibrational free energy decreases with the increase of the temperature, and the entropy and the heat capacity are proportional to the temperature and inversely proportional to the pressure. As the pressure increases, the resistance to the external pressure is strengthened for Th_4H_(15) and ThH_2.展开更多
The elastic properties and point defects of thorium monocarbide(ThC) have been studied by means of density functional theory based on the projector-augmented-wave method. The calculated electronic and elastic proper...The elastic properties and point defects of thorium monocarbide(ThC) have been studied by means of density functional theory based on the projector-augmented-wave method. The calculated electronic and elastic properties of ThC are in good agreement with experimental data and previous theoretical results. Five types of point defects have been considered in our study, including the vacancy defect, interstitial defect, antisite defect, schottky defect, and composition-conserving defect. Among these defects, the carbon vacancy defect has the lowest formation energy of 0.29 eV. The second most stable defect(0.49 eV) is one of composition-conserving defects in which one carbon is removed to another carbon site forming a C2 dimer. In addition, we also discuss several kinds of carbon interstitial defects, and predict that the carbon trimer configuration may be a transition state for a carbon dimer diffusion in Th C.展开更多
The advantages of once-through molten salt reactors include readily available fuel,low nuclear proliferation risk,and low technical difficulty.It is potentially the most easily commercialized fuel cycle mode for molte...The advantages of once-through molten salt reactors include readily available fuel,low nuclear proliferation risk,and low technical difficulty.It is potentially the most easily commercialized fuel cycle mode for molten salt reactors.However,there are some problems in the parameter selection of once-through molten salt reactors,and the relevant burnup optimization work requires further analysis.This study examined once-through graphitemoderated molten salt reactor using enriched uranium and thorium.The fuel volume fraction(VF),initial heavy nuclei concentration(HN_(0)),feeding uranium enrichment(E_(FU)),volume of the reactor core,and fuel type were changed to obtain the optimal conditions for burnup.We found an optimal region for VF and HN_(0) in each scheme,and the location and size of the optimal region changed with the degree of E_(FU),core volume,and fuel type.The recommended core schemes provide a reference for the core design of a once-through molten salt reactor.展开更多
The activity levels of long-lived radionuclides in minerals have received more and more concern for the public health. The inductively coupled plasma mass spectrometry was used to measure the content of uranium and th...The activity levels of long-lived radionuclides in minerals have received more and more concern for the public health. The inductively coupled plasma mass spectrometry was used to measure the content of uranium and thorium in 60 mineral samples collected from 16 mines of seven provinces in China. The contents of uranium and thorium ranged0.17 ± 0.04 lg g^(-1)to 15.3 ± 2.39 lg g^(-1), and 0.19 ± 0.04 lg g^(-1)to 19.6 ± 7.56 lg g^(-1), respectively. The highest levels of U and Th contents were found in aluminum ore,whereas the lowest was found in antimony and copper ores.展开更多
The molten salt reactor(MSR), as one of the Generation Ⅳ advanced nuclear systems, has attracted a worldwide interest due to its excellent performances in safety, economics, sustainability, and proliferation resistan...The molten salt reactor(MSR), as one of the Generation Ⅳ advanced nuclear systems, has attracted a worldwide interest due to its excellent performances in safety, economics, sustainability, and proliferation resistance. The aim of this work is to provide and evaluate possible solutions to fissile 233 U production and further the fuel transition to thorium fuel cycle in a thermal MSR by using plutonium partitioned from light water reactors spent fuel. By using an in-house developed tool, a breeding and burning(B&B) scenario is first introduced and analyzed from the aspects of the evolution of main nuclides, net 233 U production, spectrum shift, and temperature feedback coefficient. It can be concluded that such a Th/Pu to Th/^(233)U transition can be accomplished by employing a relatively fast fuel reprocessing with a cycle time less than 60 days. At the equilibrium state, the reactor can achieve a conversion ratio of about 0.996 for the 60-day reprocessing period(RP) case and about 1.047 for the 10-day RP case.The results also show that it is difficult to accomplish such a fuel transition with limited reprocessing(RP is 180 days),and the reactor operates as a converter and burns the plutonium with the help of thorium. Meanwhile, a prebreeding and burning(PB&B) scenario is also analyzed briefly with respect to the net 233 U production and evolution of main nuclides. One can find that it is more efficient to produce 233 U under this scenario, resulting in a double time varying from about 1.96 years for the 10-day RP case to about 6.15 years for the 180-day RP case.展开更多
Fertile fuel, such as thorium or depleted uranium, can be bred into fissile fuel and burnt in a breed-andburn(B&B) reactor. Modeling a full core with fertile fuel can assess the performance of a B&B reactor wi...Fertile fuel, such as thorium or depleted uranium, can be bred into fissile fuel and burnt in a breed-andburn(B&B) reactor. Modeling a full core with fertile fuel can assess the performance of a B&B reactor with exact quantitative estimates, but costs too much computation time. For simplicity, performing the recently developed neutron balance method with a zero-dimensional(0-D)model can also provide a reasonable result. Based on the0-D model, the feasibility of the B&B mode for thorium fuel in a fast reactor cooled by sodium was investigated by considering the(n, 2n) and(n, 3n) reaction rates of fuel and coolant in this work, and compared with that of depleted uranium fuel. Afterward, the performance of the same thorium-based fuel core, but cooled by helium, lead-bismuth, and FLi Be, respectively, is discussed. It is found that the(n, 2n) and(n, 3n) reactions should not be neglected for the neutron balance calculation for thorium-based fuel to sustain the B&B mode of operation.展开更多
To develop a microbe-based bioremediation strategy for cleaning up thorium-contaminated sites, we have investigated the biosorption behavior and mechanism of thorium on Bacillus sp. dwc-2, one of the dominant species ...To develop a microbe-based bioremediation strategy for cleaning up thorium-contaminated sites, we have investigated the biosorption behavior and mechanism of thorium on Bacillus sp. dwc-2, one of the dominant species of bacterial groups isolated from soils in Southwest China. Thorium biosorption depended on the p H of environment, and its rapid biosorption reached a maximum of up to 10.75 mg Th per gram of the bacteria(wet wt.) at pH 3.0. The biosorption agreed bettter with Langmuir isotherm model than Freundlich model, indicating that thorium biosorption was a monolayer adsorption. The thermodynamic parameters, negative change in Gibbs free energy and positive value in enthalpy and entropy, suggested that the biosorption was spontaneous,more favorable at higher temperature and endothermic process with an increase of entropy. Scanning electron microscopy(SEM) indicated that thorium initially binded with the cell surface, while transmission electron microscopy(TEM) revealed that Th deposited in the cytoplasm and served as cores for growth of element precipitation(e.g., phosphate minerals) or by self-precipitation of hydroxides, which is probably controlled by ion-exchange, as evidenced by particle induced X-ray emission(PIXE) and enhanced proton backscattering spectrometry(EPBS). Fourier Transform Infrared(FTIR) further indicated that thorium biosorption involved carboxyl and phosphate groups and protein in complexation or electrostatic interaction. Overall results indicated that a combined electrostatic interaction-complexation-ion exchange mechanism could be involved in thorium biosorption by Bacillus sp. dwc-2.展开更多
To isolate and separate thorium from nitric acid solutions, three silica-based anion exchange resins were synthesized. Batch experiments were carried out to investigate adsorption behavior of thorium in nitric acid so...To isolate and separate thorium from nitric acid solutions, three silica-based anion exchange resins were synthesized. Batch experiments were carried out to investigate adsorption behavior of thorium in nitric acid solutions. Adsorption at different concentrations of nitric acid and thorium, influence of contact time and coexisting metal ions, and effect of NO3– were investigated in detail. It was found that at high HNO3 concentrations,the resins exhibited higher adsorption capacity and better affinity towards thorium. The adsorption kinetics could be described by the pseudo-second order model equation, while the adsorption isotherms were well correlated by the Langmuir model. The maximum capacity towards thorium species on SiPyR-N4 was evaluated at 27–28 mg/g-resin. The thermodynamic parameters indicated the adsorption was an exothermic reaction. The presence of NO3– was found to promote the retention of the thorium species.展开更多
To fabricate thorium-based fuel kernel for solid fuel molten salt reactor,a component of tri-structural isotropic fuel particles is mostly based on sol-gel method.The preparation of thorium sol is an important step fo...To fabricate thorium-based fuel kernel for solid fuel molten salt reactor,a component of tri-structural isotropic fuel particles is mostly based on sol-gel method.The preparation of thorium sol is an important step for fabrication of thorium-based fuel kernels,such as thorium carbide and thorium oxide.The gel quality affects the gel particle dispersion and the final products.In this work,thorium sols were prepared using Th(NO_3)_4 and NH_3·H_2O by sol-gel method.The effects of thorium concentration,mole ratio of NH_4^+/NO_3^- and reaction temperature on the pH,viscosity,turbidity,particle size and the thorium sol distribution were investigated.The results show that the viscosity and turbidity increased with the NH_4^+/NO_3^- ratio;the turbidity and colloidal particle size increased with the reaction temperature,which affected little the sol viscosity;the sol viscosity increased with the thorium concentration,which virtually did not change the turbidity;and the particle size decreased and the size distribution narrowed with increasing thorium concentration.The sol could be stored at room temperature for one day without significant property changes.Thorium gel spheres of good quality were prepared at 60℃ with the NH_4^+/NO_3^- ratio of 75-85% and the thorium concentration of 1.2-1.4 mol/L.展开更多
A new kind of diamide N,N,N’,N’-tetrahexylsuccinylamide(THSA) was synthesized, characterized and used for the extraction of HNO3, U(VI) and TI(IV) in a diluent composed of 0.5 volume fraction 1,2,4-trimethy be...A new kind of diamide N,N,N’,N’-tetrahexylsuccinylamide(THSA) was synthesized, characterized and used for the extraction of HNO3, U(VI) and TI(IV) in a diluent composed of 0.5 volume fraction 1,2,4-trimethy benzene(TMB) and 0.5 volume fraction kerosene(OK). Extraction distribution coefficients of U(VI) and TI(IV) as functions of aque- ous nitric acid concentration, extractant concentration, temperature and salting-out agent (LiNO3 ) have been studied, and it is found that THSA as an extractant is superior to TBP for extraction of U(VI) and TI(IV). Back extraction was also studied. At low acidity, the main adduct of THSA and HNO3 is HNO3.THSA. THSA.(HNO3)2 and THSA.(HNO3)3 are also found at high acidity. The compositions of extracted species, apparent equilibrium constants and enthalpies of extraction reactions have also been calculated.展开更多
基金supported by the National Natural Science Foundation of China(Nos.11535009 and 51406114)
文摘Axial gas-liquid separators have been adopted in fission gas removal systems for the development of thorium molten salt reactors. In our previous study, we observed an unsteady flow phenomenon in which the flow pattern is directly dependent on the backpressure in a gas-liquid separator; however, the underlying flow mechanism is still unknown. In order to move a step further in clarifying how the flow pattern evolves with a variation in backpressure, a large eddy simulation(LES) was adopted to study the flow field evolution. In the simulation, an artificial boundary was applied at the separator outlet under the assumption that the backpressure increases linearly. The numerical results indicate that the unsteady flow feature is captured by the LES approach, and the flow transition is mainly due to the axial velocity profile redistribution induced by the backpressure variation. With the increase in backpressure,the axial velocity near the downstream orifice transits from negative to positive. This change in the axial velocity sign forces the unstable spiral vortex to become a stable rectilinear vortex.
文摘This work presents the results of computer simulation of neutronic processes in a high-temperature gas-cooled thorium reactor for 30 different options of core loading.To guarantee stable and long-term reactor operation(7-10 years),the quantity of fuel compact dispersion phase and starting fuel composition was selected.It is demonstrated that it is possible in principle to substitute the near-axial recirculation zone of the reactor core by a long magnetic trap with a high-temperature plasma column for generating thermonuclear neutrons.The distribution of neutron yield along the length of the plasma source is also presented.Such a thorium reactor,with a near-axial source of extra neutrons,can be applied for researching thermophysical and neutronic characteristics of dispersion thorium fuel to improve its properties.The results of the work are of great interest from the perspective of future advancement of the thermonuclear power industry,by means of creation of a hybrid installation based on a thorium reactor with a long plasma column as a source of additional neutrons.
基金supported by the Chinese TMSR Strategic Pioneer Science and Technology Project(No.XDA02010000)the Frontier Science Key Program of the Chinese Academy of Sciences(No.QYZDY-SSW-JSC016)
文摘Herein, we assess the129I transmutation capability of a 2250-MWt single-fluid double-zone thorium molten salt reactor(SD-TMSR) by considering two methods. One is realized by loading an appropriate amount of129I before the startup of the reactor, and the amount of129I during operation is kept constant by online feeding129I.The other adopts only an initial loading of129I before startup, and no other129I is fed online during operation.The investigation first focuses on the effect of the loading of I on the Th-233U isobreeding performance. The results indicate that a233U isobreeding mode can be achieved for both scenarios for a 60-year operation when the initial molar proportion of LiI is maintained within 0.40% and 0.87%, respectively. Then, the transmutation performances for the two scenarios are compared by changing the amount of injected iodine into the core. It is found that the scenario that adopts an initial loading of129I shows a slightly better transmutation performance in comparison with the scenario that adopts online feeding of129I when the net233U productions for the two scenarios are kept equal. The initial loading of129I scenario with LiI = 0.87% molar proportion is recommended for129I transmutation in the SD-TMSR,and can transmute 1.88 t of129I in the233U isobreeding mode over 60 years.
基金Project supported by the Long-Term Subsidy Mechanism from the Ministry of Finance and the Ministry of Education of China
文摘The high pressure behaviors of Th_4H_(15) and ThH_2 are investigated by using the first-principles calculations based on the density functional theory(DFT). From the energy–volume relations, the bct phase of ThH_2 is more stable than the fcc phase at ambient conditions. At high pressure, the bct ThH_2 and bcc Th_4H(15) phases are more brittle than they are at ambient pressure from the calculated elastic constants and the Poisson ratio. The thermodynamic stability of the bct phase ThH_2 is determined from the calculated phonon dispersion. In the pressure domain of interest, the phonon dispersions of bcc Th_4H(15) and bct ThH_2 are positive, indicating the dynamical stability of these two phases, while the fcc ThH_2 is unstable. The thermodynamic properties including the lattice vibration energy, entropy, and specific heat are predicted for these stable phases. The vibrational free energy decreases with the increase of the temperature, and the entropy and the heat capacity are proportional to the temperature and inversely proportional to the pressure. As the pressure increases, the resistance to the external pressure is strengthened for Th_4H_(15) and ThH_2.
基金Project supported by the International S&T Cooperation Program of China(Grant No.2014DFG60230)the National Natural Science Foundation of China(Grant No.91326105)+1 种基金the National Basic Research Program of China(Grant No.2010CB934504)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA02040104)
文摘The elastic properties and point defects of thorium monocarbide(ThC) have been studied by means of density functional theory based on the projector-augmented-wave method. The calculated electronic and elastic properties of ThC are in good agreement with experimental data and previous theoretical results. Five types of point defects have been considered in our study, including the vacancy defect, interstitial defect, antisite defect, schottky defect, and composition-conserving defect. Among these defects, the carbon vacancy defect has the lowest formation energy of 0.29 eV. The second most stable defect(0.49 eV) is one of composition-conserving defects in which one carbon is removed to another carbon site forming a C2 dimer. In addition, we also discuss several kinds of carbon interstitial defects, and predict that the carbon trimer configuration may be a transition state for a carbon dimer diffusion in Th C.
基金supported by the Shanghai Sailing Program(No.19YF1457900)Chinese TMSR Strategic Pioneer Science and Technology Project(No.XDA02010000)+1 种基金National Natural Science Foundation of China(No.12005290)Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2020261)。
文摘The advantages of once-through molten salt reactors include readily available fuel,low nuclear proliferation risk,and low technical difficulty.It is potentially the most easily commercialized fuel cycle mode for molten salt reactors.However,there are some problems in the parameter selection of once-through molten salt reactors,and the relevant burnup optimization work requires further analysis.This study examined once-through graphitemoderated molten salt reactor using enriched uranium and thorium.The fuel volume fraction(VF),initial heavy nuclei concentration(HN_(0)),feeding uranium enrichment(E_(FU)),volume of the reactor core,and fuel type were changed to obtain the optimal conditions for burnup.We found an optimal region for VF and HN_(0) in each scheme,and the location and size of the optimal region changed with the degree of E_(FU),core volume,and fuel type.The recommended core schemes provide a reference for the core design of a once-through molten salt reactor.
基金financial support by the Chinese Ministry of Science and Technology (Grant Nos. 2005DIB1J087, 2013BAK03B00)
文摘The activity levels of long-lived radionuclides in minerals have received more and more concern for the public health. The inductively coupled plasma mass spectrometry was used to measure the content of uranium and thorium in 60 mineral samples collected from 16 mines of seven provinces in China. The contents of uranium and thorium ranged0.17 ± 0.04 lg g^(-1)to 15.3 ± 2.39 lg g^(-1), and 0.19 ± 0.04 lg g^(-1)to 19.6 ± 7.56 lg g^(-1), respectively. The highest levels of U and Th contents were found in aluminum ore,whereas the lowest was found in antimony and copper ores.
基金supported by the Chinese TMSR Strategic Pioneer Science and Technology Project(No.XDA02010000)the National Natural Science Foundation of China(No.91326201)the Frontier Science Key Program of the Chinese Academy of Sciences(No.QYZDY-SSW-JSC016)
文摘The molten salt reactor(MSR), as one of the Generation Ⅳ advanced nuclear systems, has attracted a worldwide interest due to its excellent performances in safety, economics, sustainability, and proliferation resistance. The aim of this work is to provide and evaluate possible solutions to fissile 233 U production and further the fuel transition to thorium fuel cycle in a thermal MSR by using plutonium partitioned from light water reactors spent fuel. By using an in-house developed tool, a breeding and burning(B&B) scenario is first introduced and analyzed from the aspects of the evolution of main nuclides, net 233 U production, spectrum shift, and temperature feedback coefficient. It can be concluded that such a Th/Pu to Th/^(233)U transition can be accomplished by employing a relatively fast fuel reprocessing with a cycle time less than 60 days. At the equilibrium state, the reactor can achieve a conversion ratio of about 0.996 for the 60-day reprocessing period(RP) case and about 1.047 for the 10-day RP case.The results also show that it is difficult to accomplish such a fuel transition with limited reprocessing(RP is 180 days),and the reactor operates as a converter and burns the plutonium with the help of thorium. Meanwhile, a prebreeding and burning(PB&B) scenario is also analyzed briefly with respect to the net 233 U production and evolution of main nuclides. One can find that it is more efficient to produce 233 U under this scenario, resulting in a double time varying from about 1.96 years for the 10-day RP case to about 6.15 years for the 180-day RP case.
基金supported by the Chinese TMSR Strategic Pioneer Science and Technology Project(No.XDA02010000)
文摘Fertile fuel, such as thorium or depleted uranium, can be bred into fissile fuel and burnt in a breed-andburn(B&B) reactor. Modeling a full core with fertile fuel can assess the performance of a B&B reactor with exact quantitative estimates, but costs too much computation time. For simplicity, performing the recently developed neutron balance method with a zero-dimensional(0-D)model can also provide a reasonable result. Based on the0-D model, the feasibility of the B&B mode for thorium fuel in a fast reactor cooled by sodium was investigated by considering the(n, 2n) and(n, 3n) reaction rates of fuel and coolant in this work, and compared with that of depleted uranium fuel. Afterward, the performance of the same thorium-based fuel core, but cooled by helium, lead-bismuth, and FLi Be, respectively, is discussed. It is found that the(n, 2n) and(n, 3n) reactions should not be neglected for the neutron balance calculation for thorium-based fuel to sustain the B&B mode of operation.
基金Supported by National Natural Science Foundation of China(Nos.21071102 and 91126013)Joint Funds of China National Natural Science Foundation and China Academy of Engineering Physics(No.U1330125)the National Fund of China for Fostering Talents in Basic Science(No.J1210004)
文摘To develop a microbe-based bioremediation strategy for cleaning up thorium-contaminated sites, we have investigated the biosorption behavior and mechanism of thorium on Bacillus sp. dwc-2, one of the dominant species of bacterial groups isolated from soils in Southwest China. Thorium biosorption depended on the p H of environment, and its rapid biosorption reached a maximum of up to 10.75 mg Th per gram of the bacteria(wet wt.) at pH 3.0. The biosorption agreed bettter with Langmuir isotherm model than Freundlich model, indicating that thorium biosorption was a monolayer adsorption. The thermodynamic parameters, negative change in Gibbs free energy and positive value in enthalpy and entropy, suggested that the biosorption was spontaneous,more favorable at higher temperature and endothermic process with an increase of entropy. Scanning electron microscopy(SEM) indicated that thorium initially binded with the cell surface, while transmission electron microscopy(TEM) revealed that Th deposited in the cytoplasm and served as cores for growth of element precipitation(e.g., phosphate minerals) or by self-precipitation of hydroxides, which is probably controlled by ion-exchange, as evidenced by particle induced X-ray emission(PIXE) and enhanced proton backscattering spectrometry(EPBS). Fourier Transform Infrared(FTIR) further indicated that thorium biosorption involved carboxyl and phosphate groups and protein in complexation or electrostatic interaction. Overall results indicated that a combined electrostatic interaction-complexation-ion exchange mechanism could be involved in thorium biosorption by Bacillus sp. dwc-2.
基金Supported by the National Natural Science Foundation of China(No.91026019)
文摘To isolate and separate thorium from nitric acid solutions, three silica-based anion exchange resins were synthesized. Batch experiments were carried out to investigate adsorption behavior of thorium in nitric acid solutions. Adsorption at different concentrations of nitric acid and thorium, influence of contact time and coexisting metal ions, and effect of NO3– were investigated in detail. It was found that at high HNO3 concentrations,the resins exhibited higher adsorption capacity and better affinity towards thorium. The adsorption kinetics could be described by the pseudo-second order model equation, while the adsorption isotherms were well correlated by the Langmuir model. The maximum capacity towards thorium species on SiPyR-N4 was evaluated at 27–28 mg/g-resin. The thermodynamic parameters indicated the adsorption was an exothermic reaction. The presence of NO3– was found to promote the retention of the thorium species.
基金supported by the Strategic Priority Program of the Chinese Academy of Sciences(Nos.XDA 02030000 and XDA02030200)the Frontier Science Key Program of the Chinese Academy of Sciences(No.QYZDY-SSW-JSC016)
文摘To fabricate thorium-based fuel kernel for solid fuel molten salt reactor,a component of tri-structural isotropic fuel particles is mostly based on sol-gel method.The preparation of thorium sol is an important step for fabrication of thorium-based fuel kernels,such as thorium carbide and thorium oxide.The gel quality affects the gel particle dispersion and the final products.In this work,thorium sols were prepared using Th(NO_3)_4 and NH_3·H_2O by sol-gel method.The effects of thorium concentration,mole ratio of NH_4^+/NO_3^- and reaction temperature on the pH,viscosity,turbidity,particle size and the thorium sol distribution were investigated.The results show that the viscosity and turbidity increased with the NH_4^+/NO_3^- ratio;the turbidity and colloidal particle size increased with the reaction temperature,which affected little the sol viscosity;the sol viscosity increased with the thorium concentration,which virtually did not change the turbidity;and the particle size decreased and the size distribution narrowed with increasing thorium concentration.The sol could be stored at room temperature for one day without significant property changes.Thorium gel spheres of good quality were prepared at 60℃ with the NH_4^+/NO_3^- ratio of 75-85% and the thorium concentration of 1.2-1.4 mol/L.
文摘A new kind of diamide N,N,N’,N’-tetrahexylsuccinylamide(THSA) was synthesized, characterized and used for the extraction of HNO3, U(VI) and TI(IV) in a diluent composed of 0.5 volume fraction 1,2,4-trimethy benzene(TMB) and 0.5 volume fraction kerosene(OK). Extraction distribution coefficients of U(VI) and TI(IV) as functions of aque- ous nitric acid concentration, extractant concentration, temperature and salting-out agent (LiNO3 ) have been studied, and it is found that THSA as an extractant is superior to TBP for extraction of U(VI) and TI(IV). Back extraction was also studied. At low acidity, the main adduct of THSA and HNO3 is HNO3.THSA. THSA.(HNO3)2 and THSA.(HNO3)3 are also found at high acidity. The compositions of extracted species, apparent equilibrium constants and enthalpies of extraction reactions have also been calculated.