Cross section measurements for (n, p) and (n, 2n) reactions of rare-earth isotopes at neutron energies from 13.5 to 14.6 MeV

Cross sections for (n, p) and (n, 2n) reactions have been measured on some rare-earth isotopes at neutron energies of 13.5-14.6 MeV using activation technique. Data are reported for the following reactions:¹⁵⁰Nd(n, 2n) ¹⁴⁹Nd, ¹⁴⁸Nd(n, 2n) ¹⁴⁷Nd, ¹⁴²Nd(n, 2n) ¹⁴¹Nd, ¹⁶⁰Gd(n, 2n) ¹⁵⁹Gd, ¹⁵⁸Gd(n, p) ¹⁵⁸Eu, ¹⁴⁶Nd(n, p) ¹⁴⁶Pr, ¹⁴¹Pr(n, p) ¹⁴¹Ce and ¹³⁹La(n, p) ¹³⁹Ba. The neutron fluences are determined by the cross sections of ²⁷Al(n, a) ²⁴Na and ⁹³Nb(n, 2n) ^92mNb reactions. This revised version was published online in August 2006 with corrections to the Cover Date.     

Isomeric yield ratios for the natNd(γ, xn) 139m,g; 141m,gNd reactions in the bremsstrahlung energy region from 45 to 60 MeV

The independent isomeric yield ratios (IR) for the ^139m,gNd and the ^141m,gNd isomeric pairs produced from the ^natNd(γ, xn) reactions were determined by the activation and the off-line γ-ray spectrometric technique at the end-point bremsstrahlung energies of 45, 50, 55, and 60 MeV in the 100 MeV electron Linac of the Pohang accelerator laboratory, Korea. The present IR for the ^141m,gNd isomeric pair were compared with those from the literature measured by the bremsstrahlung and the neutron to examine the role of excitation energy. The obtained IR for the ^139m,gNd and the ^141m,gNd isomeric pairs from ^natNd(γ, xn) reactions were compared with those from the ¹⁴¹Pr(p, x), the ^natCe(³He, x), and the ¹³⁶Ce(α, n) reactions to examine the role of parameters in entrance channel i.e. excitation energy and the effect of the input angular momentum. The present IR of ^139m,gNd and ^141m,gNd were compared with those calculated by using the TALYS 1.4 code as well as those from the literature data of above mentioned reactions.     

Practicality of the cyclotron production of radiolanthanide 142Pr: a potential for therapeutic applications and biodistribution studies

Radiolanthanide praseodymium-142 (T _1/2 = 19.12 h, E _?? ^?  = 2.162 MeV (96.3%), E?? = 1575 keV (3.7%)) due to its high ??-emission and low specific ??-emission could not only be a therapeutic radionuclide, but also a suitable radionuclide in order for biodistribution studies. Conventionally, ¹⁴²Pr produces via ¹⁴¹Pr(n,??)¹⁴²Pr reaction by irradiation in a low-fluence reactor and this study evaluates cyclotron reaction production of it. ¹⁴²Pr excitation function via ^natLa(??,n)¹⁴²Pr, ¹⁴²Ce(p,n)¹⁴²Pr, and ^natPr(d,p)¹⁴²Pr reactions were calculated by TALYS-1.2 and EMPIRE-2.19beta codes, and with the data taken from the TENDL-2010 database. In addition, we compared them with the reported measurement by experimental data. Requisite thickness of targets was obtained by SRIM-2010 code for each reaction. The ¹⁴²Pr production yield was evaluated with attention to excitation function and stopping power. Similar to reactor produced ¹⁴²Pr; ¹⁴¹Pr impurity exists in cyclotron produced ¹⁴²Pr while it could not be separated by chemical methods. Therefore, cyclotron and reactor produced ¹⁴²Pr will be in carrier added form.     

Separation of Rare-Earth Elements from Nitrate Solutions by Solvent Extraction Using Mixtures of Methyltri-n-octylammonium Nitrate and Tri-n-butyl Phosphate

The article presents data on the solvent extraction separation of rare-earth elements (REEs), such as La(III), Ce(III), Pr(III), and Nd(III), using synergic mixtures of methyltrioctylammonium nitrate (TOMANO₃) with tri-n-butyl phosphate (TBP) from weakly acidic nitrate solutions. Specifically, experimental results on separation of REEs, for the pair Ce(III)/Pr(III) for quaternary mixtures of REEs (La(III), Ce(III), Pr(III), Nd(III)) and for the pair La(III)/Pr(III) for solutions containing La(III), Pr(III), and Nd(III), are presented. It was shown that effective separation for the pair Ce(III)/Pr(III) from a solution containing 219 g Ce(III)/L, 106 g La(III)/L, 20 g Pr(III)/L, 55 g Nd(III)/L, and 0.1 mol/L HNO₃, was achieved using 56 steps of a multistage, counter-current solvent extraction cascade with scrubbing, at an organic-to-aqueous phase volume ratio (O/A) equal to 2/1 on the extraction section and O/A equal to 4/1 on the scrubbing section, using 3.3 mol/L solutions of the mixture TOMANO₃-TBP with molar ratio 0.15:0.85 in dodecane. Separation for the pair La(III)/Pr(III) could be achieved using a solvent extraction cascade with scrubbing in 32 steps at O/A equal to 2/1 on the extraction section and O/A equal to 2.8/1 on the scrubbing section of the solvent extraction cascade from a solution containing 258 g La(III)/L, 58 g Pr(III)/L, 141 g Nd(III)/L, and 0.1 mol/L HNO₃ with 3.0 mol/L solution of the mixture TOMANO₃-TBP with molar ratio 0.2:0.8 in dodecane.     

Excitation functions of neutrons induced reactions on terbium from threshold to 20 MeV

Cross-sections for (n,2n), (n,p), and (n,α) reactions have been measured on terbium isotopes at the neutron energies from 13.5 to 14.8 MeV using the activation technique in combination with high-resolution gamma-ray spectroscopy. Data are reported for the following reactions: ¹⁵⁹Tb(n,2n)^158m+gTb, ¹⁵⁹Tb(n,p)¹⁵⁹Gd, and ¹⁵⁹Tb(n,α)¹⁵⁶Eu. The cross sections were also estimated with the TALYS-1.4 nuclear model code, at neutron energies varying from the reaction threshold to 20 MeV. The results were discussed and compared with experimental data found in the literature, and with the comprehensive evaluation data in ENDF/B-VII.1 and JENDL-4.0 libraries.     

Measurement of neutron-induced activation cross sections of lanthanum at 14.8 MeV

Cross-sections for (n,p), (n,α), (n,n′α), (n,t) and (n,2p) reactions have been measured on ¹³⁹La isotope at the neutron energy 14.8 MeV using the activation technique in combination with high-resolution gamma-ray spectroscopy. Neutrons were produced via the ³H(d,n)⁴He reaction using a solid tritium–titanium target. The neutron fluences were determined using the monitor reaction ²⁷Al(n,α)²⁴Na. The neutron energy in this measurement was determined by cross section ratios for the ⁹⁰Zr(n,2n)^89m+gZr and ⁹³Nb(n,2n)^92mNb reactions. Data are reported for the following reactions: ¹³⁹La(n,p)¹³⁹Ba, ¹³⁹La(n,α)¹³⁶Cs, ¹³⁹La(n,n′α)^135mCs, ¹³⁹La (n,t)^137mBa, and ¹³⁹La(n,2p)¹³⁸Cs. The cross sections were discussed and compared with experimental data found in the literature, and with the comprehensive evaluation data in ENDF/B-VII.0, JENDL-3.3, JEFF-3.1/A, and TENDL-2008 libraries.     

Channel effect in isomeric ratio of 137m,gCe produced in different nuclear reactions

This work presents the experimental study of the isomeric ratio of ^137mCe–^137gCe produced in ¹³⁸Ce(γ, n) ^137m,gCe photonuclear reaction, in neutron capture reaction ¹³⁶Ce(n, γ) ^137m,gCe and in the two simultaneous reactions ¹³⁸Ce(γ, n) ^137m,gCe and ¹³⁶Ce(n, γ) ^137m,gCe in the mixed photon—neutron field by the activation method. The investigated samples were irradiated at the bremsstrahlung photon flux, in the epithermal and thermal-epithermal neutron beam and in the mixed photon-neutron field constructed at the electron accelerator Microtron MT-25 of the Flerov Laboratory of Nuclear Reaction, Joint Institute for Nuclear Research, Dubna, Russia. The results were analyzed, discussed and compared with those of other authors to examine the role of the channel effect in nuclear reaction and provide the nuclear data for theoretical model interpretation of nuclear reactions.

     

Lanthanoid‐Based Ionic Liquids Incorporating the Dicyanonitrosomethanide Anion

A series of low‐melting‐point salts with hexakisdicyanonitrosomethanidolanthanoidate anions has been synthesised and characterised: (C₂mim)₃[Ln(dcnm)₆] ( 1 Ln ; 1 Ln = 1 La , 1 Ce , 1 Pr , 1 Nd ), (C₂C₁mim)₃[Pr(dcnm)₆] ( 2 Pr ), (C₄C₁pyr)₃[Ce(dcnm)₆] ( 3 Ce ), (N₁₁₁₄)₃[Ln(dcnm)₆] ( 4 Ln ; 4 Ln = 4 La , 4 Ce , 4 Pr , 4 Nd , 4 Sm , 4 Gd ), and (N_1112OH)₃[Ce(dcnm)₆] ( 5 Ce ) (C₂mim=1‐ethyl‐3‐methylimidazolium, C₂C₁mim=1‐ethyl‐2,3‐dimethylimidazolium, C₄C₁py=N‐butyl‐4‐methylpyridinium, N₁₁₁₄=butyltrimethylammonium, N_1112OH=2‐(hydroxyethyl)trimethylammonium=choline). X‐ray crystallography was used to determine the structures of complexes 1 La , 2 Pr , and 5 Ce , all of which contain [Ln(dcnm)₆]^3? ions. Complexes 1 Ln and 2 Pr were all ionic liquids (ILs), with complex 3 Ce melting at 38.1 °C, the lowest melting point of any known complex containing the [Ln(dcnm)₆]^3? trianion. The ammonium‐based cations proved to be less suitable for forming ILs, with complexes 4 Sm and 4 Gd being the only salts with the N₁₁₁₄ cation to have melting points below 100 °C. The choline‐containing complex 5 Ce did not melt up to 160 °C, with the increase in melting point possibly being due to extensive hydrogen bonding, which could be inferred from the crystal structure of the complex.     

Cross-section calculations of proton induced (p,n) and (p,2n) reactions for production of diagnostic 67Ga, 81Rb, 111In, 123,124I, 123Cs and 123Xe radioisotopes

Investigation of pre-equilibrium (PEQ) and equilibrium (EQ) effects on proton induced reactions for production of radioisotopes are very important. Therefore, in this study, we have calculated the PEQ and EQ cross-sections for ⁶⁷Zn(p,n)⁶⁷Ga, ⁶⁸Zn(p,2n)⁶⁷Ga, ⁸²Kr(p,2n)⁸¹Rb, ¹¹¹Cd(p,n)¹¹¹In, ¹¹²Cd(p,2n)¹¹¹In, ¹²³Te(p,n)¹²³I, ¹²⁴Te(p,2n)¹²³I, ¹²⁴Te(p,n)¹²⁴I and ¹²⁴Xe(p,2n)¹²³Cs reactions for production diagnostic radioisotopes. Calculations have been performed by using the hybrid model, geometry dependent hybrid model and full exciton model of PEQ reaction mechanism with 1–40 MeV proton incident energy. We have also investigated the EQ effects on these reactions using the Weisskopf–Ewing model in the same energy range. The excitation functions including the PEQ and EQ effects on these reactions are evaluated by using the ALICE/ASH (2006) and the TALYS 1.4 (2011) codes. Our results have shown that using these codes is suitable for production diagnostic isotopes mentioned above. To obtain excitation functions for producing the diagnostic radioisotopes the PEQ mechanism has been found more dominant than that of the EQ. The results are discussed and compared with the available experimental data.     

XPS study of the surface properties and Ni particle size determination of Ni‐supported catalysts

The surface properties of Ni/MgAl₂O₄ catalysts doped with Ce or Pr were analyzed by XPS after treatment in an inert and reductive atmosphere at 400 °C. The Ce‐promoted solids presented the Ce³⁺/Ce⁴⁺ couple on the surface even after treatment in a reductive atmosphere, H₂(5%)/Ar. The promotion effect of Ce on these solids could be associated with their participation on the carbon deposition‐removal mechanism. Pr‐doped catalysts showed a very high concentration of Pr³⁺ under a reductive atmosphere and the redox behavior associated with the carbon removal could be partially inhibited or become slower. The size of the Ni⁰ particles after both an inert and a reductive atmosphere was estimated by XPS intensity ratio using the model proposed by Davis. The results obtained from the Davis model showed that an important increase occurred in Ni particle size after treatment in H₂(5%)/Ar for the Pr‐promoted solids. The metal sintering under reductive atmosphere could be the reason for the higher loss of activity of the Pr‐doped solids under reforming conditions. Copyright © 2014 John Wiley & Sons, Ltd.     

Cross section measurements for 141Pr(n,γ)142Pr reaction at neutron energies from 13.5 to 14.8?MeV

Activation cross-sections were measured for the ¹⁴¹Pr(n,??)¹⁴²Pr reaction at three different neutron energies from 13.5 to 14.8?MeV. The fast neutrons were produced via the ³H(d,n)⁴He reaction on Pd-300 neutron generator. The natural high-purity Pr₂O₃ powder was used as target material. Induced gamma activities were measured by a high-resolution gamma-ray spectrometer with high-purity germanium detector. Measurements were corrected for gamma-ray attenuations, random coincidence (pile-up), dead time and fluctuation of neutron flux. The neutron fluences were determined by the cross section of ²⁷Al(n,??)²⁴Na reaction. The neutron energy in the measurement were by the cross section ratios of ⁹⁰Zr(n,2n)^89m+gZr and ⁹³Nb(n,2n)^92mNb reactions. The data for ¹⁴¹Pr(n,??)¹⁴²Pr reaction cross sections are reported to be 3.3?±?0.2, 2.7?±?0.2 and 2.2?±?0.2 mb at 13.5?±?0.2, 14.1?±?0.2, and 14.8?±?0.2?MeV incident neutron energies, respectively. Results were discussed and compared with some corresponding values found in the literature.     

Determination of the fast fission yield of141Pr using neutron activation analysis

A method is described for the determination of the fission yield of¹⁴¹Pr. This method was developed to determine the fast fission yield of¹⁴¹Pr in the Mark III loading (enriched uranium with about 2% zirconium) of the fast fission breeder reactor, EBR-1. The burnup of the fuel sample was determined using the previously reported fission yield of¹³⁷Cs. Praseodymium was separated from uranium, plutonium and other fission products by a combination of precipitation and ion exchange stages. Thereafter,⁵⁵Mn was added to serve as an internal flux monitor and praseodymium determined by neutron activation analysis. A precision of ±2% was obtained. Presented at the 15th Annual Meeting of the American Chemical Society, Miami Beach, Florida (USA), April 1967.     

Flame-ion chemistry of the lanthanide metals Ce,Pr and Nd

A pair of premixed, H₂O₂Ar flames of fuel-rich (FR) and fuel-lean (FL) composition, both at atmospheric pressure and 2425 K, were doped with about 10⁻⁶ mol fraction of the lanthanide metals La, Ce, Pr and Nd; from a previous study, La was used as a benchmark. The metals produce solid particles in the flames and gaseous metallic species. The latter include metallic atoms A near the flame reaction zone, but only the monoxide AO, the oxide hydroxide OAOH and, in some cases, the dioxide AO₂ further downstream at equilibrium. Metallic ions (< 1% of the total metal) were observed by sampling the flames through a nozzle into a mass spectrometer. All of the observed ions can be represented by four hydrate series: (a) major signals of AO⁺·nH₂O (n = 0–3) for La, Ce, Pr and Nd; (b) small signals of AO₂H⁺·nH₂O (n = 0–2) for Ce, Pr and Nd; (c) still smaller signals of AO₂⁺·nH₂O (n = 0, 1) for Ce, Pr and Nd in the FL flame only; and (d) tiny signals of AOH⁺·nH₂O (n = 0, 1) for Pr and Nd in the FR flame only. The actual structures of some of these ions may not correspond to simple hydrates: e.g. AO⁺·H₂O = A(OH)₂⁺ = protonated OAOH; AO₂H⁺·H₂O = A(OH)₃⁺, etc. Since hydrogen flames contain essentially no natural ionization, a major objective was to consider probable ionization mechanisms for the metals. The primary reactions include both chemi-ionization, and thermal (collisional) ionization of AO whose ionization energy is low (about 5 eV). Some of the ions are formed by secondary ion/molecule reactions including three-body hydration, proton transfer, electron (charge) transfer, H atom abstraction by radicals and oxidation. In addition, the chemical ionization of the metallic species by H₃O⁺ was investigated. The flame-ion chemistry of these metals is discussed in detail.     

Cross-sections of 14 MeV neutron reactions producing short-lived nuclides

The cross-sections for the production of the short-lived nuclides:^26mAl,^197mAu,^136mBa,^79mBr,^139mCe,³⁴Cl,^167mEr,^114m3In,^114m2In,^38mK,^38mCl,²⁶Na,²⁰F,¹⁹²Re,^207mPb,^203mPb,^46mSc,^183mW,^90mZr obtained from (n, 2n), (n, n′), (n, alpha), (n,p) reactions using 14 MeV neutrons, were evaluated by the activation method. The experimental results of this work were compared with those obtained by other authors.     

Chromatographic isolation of144Ce and144Pr from the wastes of irradiated uranium treatment

A two-step chromatographic technique was elaborated to isolate¹⁴⁴Ce,¹⁴⁴Pr from a solution of uranium fission products in 6M HNO₃. The oxidation to Ce(III) by bromate and selective adsorption of¹⁴⁴Ce(IV) on anion exchange column were used to concentrate and purify¹⁴⁴Ce. Some impurities of uranium,⁹⁵Zr,⁹⁵Nb,¹⁰⁶Ru remain in¹⁴⁴Ce solution after the first step of its isolation. The final purification is achieved by passing the 6M HNO₃ solution of¹⁴⁴Ce(IV) through the HDEHP-coated teflon column. The decontamination factors of¹⁴⁴Ce from main fission products are given. 7.2 mCi of (¹⁴⁴Ce+¹⁴⁴Pr) are recovered from each gram of irradiated uranium trioxide with the yield greater than 99%. An improvement of known generator was carried out to elute a purer¹⁴⁴Pr from maternal¹⁴⁴Ce(IV) adsorbed on the anion exchange column.     

Activation cross sections and isomeric cross section ratios for 184Os(n,2n)183m,gOs, 190Os(n,p)190m,gRe and 86Sr(n,2n)85m,gSr reactions from 13.5 to 14.8 MeV

The cross sections for the ¹⁸⁴Os(n,2n)^183m,gOs, ¹⁹⁰Os(n,p)^190m,gRe and ⁸⁶Sr(n,2n)^85m,gSr reactions and their isomeric cross section ratios σ _m /σ _g have been measured in the neutron energy range of 13.5–14.8 MeV using the activation technique. Nuclear model calculations using the code HFTT, which employs the Hauser-Feshbach (statistical model) and exciton model (precompound effects) formalisms, were undertaken to describe the formation of the products. The total cross sections for ¹⁸⁴Os(n,2n)¹⁸³Os, ¹⁹⁰Os(n,p)¹⁹⁰Re and ⁸⁶Sr(n,2n)⁸⁵Sr reactions are compared with the experimental data found in the literature, with results of published empirical formulae, with values of model calculations including the pre-equilibrium contribution, and with the evaluation data of JEFF-3.1/A or ENDF/B-VII.     

Structural Investigation of the Effect of Praseodymium in Eu1-xPrxBa2Cu3O7-δ and EuBa2-xPrxCu3O7-δ Perovskites by 151Eu and 141Pr Mössbauer Spectroscopy

¹⁵¹Eu and ¹⁴¹Pr Mössbauer spectroscopy was applied to study the effects of Pr substitution for Eu or Ba atoms in Eu_1-x Pr _x Ba₂Cu₃O_7- and EuBa_2-x Pr _x Cu₃O_7-, respectively. It was found that there exists a correlation between the ¹⁵¹Eu isomer shift and the onset temperature of the superconducting transition, independent of the location of Pr. This shows that the extra electrons provided by the Pr increase the electronic density in the copper oxide planes and in the 4f orbitals of Eu³¹, simultaneously. The polycrystalline compound EuBa_1.3Pr_0.7Cu₃O_7- has been investigated by ¹⁴¹Pr Mössbauer spectroscopy. The observed ¹⁴¹Pr isomer shift, (4.2 K) = 0.10(15) mm/s relative to PrF₃, reflects a valence state of 3+ for the Pr located at the Ba site in EuBa_1.3Pr_0.7Cu₃O_7-, being in contrast to the valence state of 3.4+ found earlier for Pr which was situated at the rare earth site. This means that the valence state of Pr substituted for Eu is different from that of Pr substituted for Ba. These results suggest that the suppression of superconductivity by Pr substituted for the rare earth atoms is a consequence of the hole filling effect.     

Cross sections for fast-neutron interaction with erbium isotopes

Cross-sections for (n,2n), (n,p), (n,α), and (n,d*) (The expression (n,d*) cross section used in this work includes a sum of (n, d), (n, np) and (n, pn) cross sections) reactions have been measured on erbium isotopes at the neutron energies from 13.5 to 14.8 MeV using the activation technique in combination with high-resolution gamma-ray spectroscopy. Data are reported for the following reactions: ¹⁶²Er(n,2n)¹⁶¹Er, ¹⁶⁴Er(n,2n)¹⁶³Er, ¹⁶⁸Er(n,α)^165mDy, ¹⁶⁶Er(n,p)^166gHo, ¹⁷⁰Er(n,α)¹⁶⁷Dy, ¹⁶⁸Er(n,p)^168m+gHo, ¹⁷⁰Er(n,p)^170gHo, and ¹⁷⁰Er(n,d*)¹⁶⁹Ho. The cross sections were discussed and compared with experimental data found in the literature, and with the comprehensive evaluation data in ENDF/B-VII.0 and l JEFF-3.1/A libraries.     

Yields and average cross sections of recoil charged particle induced reactions on11B,12C,13C,14N,16O and18O

The yield and average cross section for the reactions¹¹B(p, n)¹¹C,¹²C(p, )¹³N,¹³C(p, n)¹³N, ₁₂ ¹² C(d, n)¹³N,¹⁴N(p, )¹¹C,¹⁶O(p, )¹³N,¹⁶O(d, n)¹⁷F,¹⁶O(t, n)¹⁸F, and¹⁸O(p, n)¹⁸F have been measured in different compounds. The charged particles were created in the samples themselves either through recoil by scattering of 14 MeV neutrons off hydrogen and deuterium, or by the (n, t) reaction on⁶Li using thermal neutrons. The yields of reactions¹²C(d, n);¹⁶O(p, );¹⁶O(t, n) and¹⁸O(p, n) have been measured using proton, deuteron and triton spectra generated by 14 MeV neutrons in the reactions D(n, p)2n;⁶Li(n, d);⁷Li(n, d) and¹⁰B(n, d);⁷Li(n, t) and¹⁰B(n, t), respectively.     

Synthese und Aufbau von (4-Picolinium)[LnCl4(H2O)3] (Ln = La,Ce, Pr,Nd)

Preparation and Crystal Structure of (4-Picolinium)[LnCl₄(H₂O)₃] (Ln = La, Ce, Pr, Nd) The complex water containing chlorides (4-Picolinium)[LnCl₄(H₂O)₃] (Ln = La, Ce, Pr, Nd) were prepared for the first time, and the crystal structures of (4-Picolinium)[LnCl₄(H₂O)₃] (Ln = La, Pr) were determined on single crystals by X-ray methods. The isotypic compounds crystallize with triclinic symmetry, space group P1 , Z = 2. Surprisingly there exist the dimeric complex anions [Ln₂Cl₈(H₂O)₆]^2? (Ln = La, Pr).