Radioisotopes are widely used in the fields of medicine, science, and industry. The growing demand for medical radioisotopes has driven research on alternative production methods. In particular, both isotopes of 67Cu and 68Ge play vital roles in the medical environment in many countries to be used in the radio-immunotherapy and the positron emission tomography imaging, respectively. This study designed a multi-target system consisting of two Zn and one Ga2O3 plates to enable simultaneous production of the medical radioisotopes 67Cu and 68Ge using 100 MeV proton beams. To understand the thermal effect on the multi-targets, we examined the distribution of energy absorbed in each solid plate target when exposed to an accelerated proton beam through the thermal-fluid analysis based on ANSYS simulation. For confirming thermal stability for two Zn targets and one Ga2O3 target, the modified water flow path inside the multi-target system was designed effectively with the controlled distribution of multiple sub-holes between main inlet and the following four channels. It was confirmed that the newly designed multi-target system of Zn and Ga2O3 solid plates shows higher thermal stability than the case of uniform distribution of water inlet, which means it could be exposed to a higher current beam of 7.57% to decrease the processing time.
The rational design of binder free, non-noble, highly active, cost effective and durability of bifunctional elec-trocatalyst for efficient overall water splitting is crucial for acquiring clean hydrogen energy systems. Herein, a surface-oriented in-situ growth of molybdenum disulfide on the non-precious iron metal organic frameworks is implemented by straightforward two-step solvothermal method. The optimum Fe-MOF@MoS2-6h electrocatalyst heterostructures achieves the highly active heterointerfaces of MoS2 and Fe-MOF, facilitates the mass/charge transport of the catalyst which improves the electrical conductivity. As a consequence, the optimal Fe-MOF@-MoS2-6h achieves the lowest overpotential of-118 mV and-187 mV at 10 mA cm-2 for HER and OER, respectively, outperforming benchmark of Pt-C/NF and IrO2/NF. Moreover, an overall water splitting electro-lyzer constructed using Fe-MOF@MoS2-6h||Fe-MOF@MoS2-6h electrocatalyst, requires only a cell voltage of 1.517 V to achieve a current density of 10 mA cm-2 which is comparable to Pt-C/NF||IrO2/NF (1.588 V) water splitting device. The precisely rational designed bifunctional Fe-MOF@MoS2-6h electrode also revealed no degradation in the stability test at 50 mA cm-2 for 100 h in alkaline electrolyte. This work proposes a practical strategy for highly efficient heterointerface electrocatalysts to achieve promising electrochemical water splitting.
Ion beam irradiation is a non-destructive method to tune the composition and morphology of nanoarchitectures. It is a promising tool owing to the creation of crystal defects such as dislocations and vacancies in addition to ion implantation. Due to the advantages of structural versatility, tunability of chemical composition and high theoretical capacity, Metal organic frameworks are considered as a potential class of electrode materials for supercapacitors. We have in situ grown ZIF-67, without binder on carbon cloth and modified the interface by implanting with Ni ions. Benefiting from the Ni+ ion implanted ZIF-67 (CC/Ni@ZIF67-4) as a binder-free positive electrode delivered an areal capacitance of 1010 mF cm−2 at 1 mA cm−2 with profound cyclic retention of 93.5%. The hybrid supercapacitor assembled with CC/Ni@ZIF-67-4//CC/O,N,S@AC composition delivered a maximum voltage window of 1.5 V, exhibited a specific capacitance of 68 F g−1 at a current density of 2 Ag-1 energy density, an energy density of 21.26 Wh kg−1 and power density of 13,500 W kg−1 as well as a remarkable electrochemical stability up to 10,000 (96.4% retention at 10 Ag-1). The density functional theory calculations show a change in the Fermi level after the inclusion of Ni+ ions supporting the experimental data.
We have developed a new analytical peak separation analysis for superposed γ -ray peaks on ^67 Cu and ^67 Ga to measure the ^68 Zn( p ,2 p ) ^67 Cu and ^68 Zn( p ,2 n ) ^67 Ga reactions, unlike in most previous works that were employing a radiochemical separation to measure them. Based on the nuclear data such as the γ -ray intensity and the half-life for each nuclide, we may develop a new analytical method that enables us to estimate the respective counts arising from each nuclide, thereby obtaining the nuclear reactions. The newly developed analytical method can universally be applied to separate the superposed γ -ray spectra of any two nuclides, especially superior in separating the nuclides with different half-lives. In comparison with the data in the literature, the two reactions in the present work are in good agreement with those of some previous works. In addition, we compared the present ^68 Zn( p ,2 n ) ^67 Ga reaction without the peak separation to the data in the literature without the chemical separation, and find that a good agreement is evident, enhancing the reliability of the ^68 Zn( p , x ) ^65 Zn and ^68 Zn( p ,3 n ) ^66 Ga reactions, which are further measured in the present work
Perylene diimide (PDI)-based MOFs feature a substantial specific capacitance, terrific cycle durability, swift charge/discharge rates, exceptional chemical as well as thermal endurance, diversity in electrode design, and inexpensive production costs. In light of these benefits, PDI-based MOFs are intriguing options for utilization in energy storage. Inspired by the distinctive features of perylene diimide-based ligands, highly conjugated and nitrogen-rich organic ligands Perylene diimide-L-dopa (PDI-L-Dopa) were incorporated to create the Ni-MOF architecture. The resulting hierarchical flower-like microspheres of bi-ligand Ni-MOF had better electron transport, conductivity, and wettability. When applied as electrode material in a three-electrode system considering a specific capacitance of 198 F/g at a current density of 1 A/g, the Ni-MOF-24 h electrode showcased beneficial electrochemical efficiency. XRD, FT-IR, and XPS were used to validate the formation of Ni-MOF and disclose the exact chemical composition and valence state inside the material. The hierarchical flower-like microsphere structure of the Ni-MOF, formed of 2D petal-like nanosheets, was revealed by FE-SEM and TEM. Additionally, when Ni-MOF-24 h electrodes used to fabricate symmetric supercapacitor (SSC), it reveals a high energy density (Ed) of 23 Wh/kg at a corresponding power density (Pd) of 600 W/kg along with extraordinary cyclic stability over 10,000 charge/discharge cycles with retaining 99 % of the initial capacitance. This research sheds light on the design and manufacture of innovative materials for long-term and efficient energy storage devices based on MOFs.
Herein, we report the electrochemical energy storage performance of delta-MnO2 (K-birnessite MnO2) as super-capacitor electrode material in Na2SO4 aqueous electrolyte. The electrode exhibited considerable electrochemical performances due to the fast intercalation/deintercalation reactions of Na+ on the pseudocapacitive MnO2 surface. However, a long-term cyclic stability test of the electrode at a low specific current (1 A g(-1)) demonstrated a decline in its initial capacitance value to the tune of similar to 21%. To quantify the above discrepancy, the electrochemical intercalation of Na+ ions on the electrode surface was quantitatively studied employing electrochemical impedance spectroscopy, EDAX analysis and X-ray photoelectron spectroscopy. Further, the surface of the electrode was analyzed by performing complete charge and charge/discharge measurements at a low specific current of 0.1 A g(-1). These results disclosed that, besides the surface intercalation/deintercalation reactions, some Na+ ions have permanently substituted into the bulk (layer) of delta-MnO2 by replacing the host K ions from the layered nanostructure. Thus, this finding suggests that Na+ ions replaced in the site of K in delta-MnO2 considerably affect the electrochemical properties of the supercapacitor electrode. (C) 2021 Elsevier B.V. All rights reserved.
Bismuth selenide (Bi2Se3) is an orderly layered material with large surface area and localized surface plasmon resonance (LSPR). The electrocatalytic profile of Bi2Se3 has been least explore for energy storage applications since its pristine form is handicapped with limited electrical conductivity. Here we report an epitaxial engineering strategy to manipulate the weak van der Waals forces to expand the interlayer spacing by intercalating phosphorus (P) atom by chemical vapor deposition (CVD) method. The obtained P intercalated Bi2Se3 (P@Bi2Se3) exhibited towering LSPR, increased carrier density bestowing ample active sites, enhanced ion diffusion and plentiful channels for the exodus of electrolyte. The potential of P@Bi2Se3 was examined for energy storage application which exhibited battery like behavior with a specific capacity (C-s) of 194 C g(-1) at 3 A g(-1) current density against 121 C g(-1) by Bi2Se3/NF under identical condition and restored 88 % of its initial specific capacity even after 5000 charge/discharge cycles. The hybrid supercapacitor (HSC) assembled using P@Bi2Se3 and O, N, S@AC as positive and negative electrodes exhibited a considerable specific capacitance, high specific energy (E-s) and specific power (P-s) with excellent stability for 10000 charge/discharge cycles. The surface and interfacial engineering strategy proposed here can be extended to tune plasmonic resonance and charge carrier energy density for the successful implementation of Bi2Se3 beyond energy storage applications.
We have developed chelator-free copper-64-incorporated iron oxide (IO) nanoparticle (NPs) which have both magnetic and radioactive properties being applied to positron emission tomography (PET)-magnetic resonance imaging (MRI). We have found that the IO nanoparticles composed of radioactive isotope 64Cu may act as a contrast agent being a diagnostic tool for PET as well as a good T2 MRI nanoprobe due to their good r2/r1 ratio. Furthermore, we demonstrate that the 64Cu incorporation at the core of core-shell-structured IO NPs exhibits a good in vivo stability, giving us an insightful strategy for the design of a contrast agent for the PET-MRI system.
The development of metal-organic frameworks (MOFs) opens up a new pathway of original or sacrificial template for synthesizing unique morphologies to serve as novel supercapacitor electrode materials. Herein, we describe a synthesis of termite nest-like nanostructured manganese cobalt phosphide on carbon fiber cloth (MCP/CC) by simple wet chemical method and followed by phosphorization. The fabricated MOF-derived binder-free MCP/CC electrode unveils a maximum areal capacitance (C-a) of 338 mF cm(-2) at a current density of 2 mA cm(-2) in 6 M KOH electrolyte. Additionally, a hybrid supercapacitor (HSC) was assembled using MCP/CC as a positive electrode and N, O, S enriched activated carbon coated CC (AC@CC ) as a negative electrode, which delivered a maximum specific capacitance of 48 F g(-1) at a wide potential window of 0-1.7 V. Moreover, HSC showed an excellent specific energy and power of 19.18 Wh kg(-1) and 9996 W kg(-1) with superior capacitance retention (94%) even after 10,000 cycles. Further, the device exhibited negligible self-discharge and have good stability even after 50 h of charge holding test. These results indicate that the MCP/CC nanostructure is a favorable electrode material for highly efficient energy storage applications. (C) 2021 Published by Elsevier Ltd.
The rational design of high-performance electrodes is of major significance for the fabrication of advanced energy storage technologies. Herein, surface engineering has been extensively implemented to obtain nonprecious metal organic frameworks (MOFs) as a template, to carry out in-situ growth of iron molybdenum sulfide on nickel foam (denoted as Fe-MoS2@NF). The novel architecture of the synthesized electrode demonstrates a highperformance supercapacitor. Fe-MoS2@NF electrode delivers a high areal capacity of 3565 mC cm(-2) at a current density of 4 mA cm(-2) in 6 M KOH aqueous electrolyte and retains 89 % of areal capacity after 5000 cycles. In addition, a hybrid supercapacitor (HSC) was fabricated comprising the Fe-MoS2@NF and O, N, S@AC as positive and negative electrodes, respectively. The fabricated HSC exhibits a high specific capacity of 60 mAh g(-1) at 1 A g(-1) and delivers an excellent specific energy of 49.4 Wh kg(-1) corresponding to a specific power of 827 W kg(-1) and maintains the specific energy of 10.2 Wh kg(-1) at a high specific power of 13.42 kW kg(-1). Moreover, the device showed a better cyclic stability similar to 91 % for 10,000 charge/discharge cycles. Thus, the design concept of the electrode opens a new avenue towards the battery type supercapacitor applications.
Graphene synthesized via electrochemical exfoliation of graphite is considered to be a simple, fast, and scalable technique. This exfoliation technique leads to the formation of multi-layer graphene sheets with some defects, which is feasible for developing supercapacitor electrodes due to the presence of various pseudocapacitive functionalities. We report the exfoliation of multi-layer graphene via pulse sonication assisted electrochemical exfoliation technique (sonoelectrochemical) and studied the effect of three different aqueous electrolytes having acidic, neutral, and basic properties. The pulse (2/4) of 2 s soni-cation and 4 s rest time significantly improve the exfoliation process without hindering the electro-chemical reaction that takes place on the graphite. The structural quality and functional groups attached to the surface of the exfoliated graphene sheets were evaluated using spectroscopic techniques. The investigation reveals that the nature of electrolyte and intercalation ions highly influences the exfoliation duration, yield, size, and quality of the graphene. The graphene layers exfoliated in sulfuric acid and ammonium sulfate electrolytes possessed many defect sites than those exfoliated in KOH. However, this graphene demonstrated better electrochemical performance than the graphene exfoliated in KOH electrolyte due to the presence of various electroactive defect sites on the surface and edges of the graphene. (c) 2021 Elsevier Ltd. All rights reserved.
We investigate the magnetic properties in a frustrated spin system of carbonyl iron (CI) particles before and after Ni+ ion beam irradiation. Upon increasing temperatures, the saturation magnetization exhibits an anomalous increase, which is more intense after the beam irradiation. The zero-field cooled (ZFC) magnetization data show an anomalous increase up to 300 K, regardless of the beam irradiation. After the irradiation, unlike in the unirradiated CI particles, the ZFC curve shows separated regimes, reflecting two distributions of the blocking temperature, which may be related to the particle distribution summed with two distribution functions. After the irradiation, strong interparticle interaction may be present due to the effect of dipolar interaction among CI particles doped Ni ions, leading to the enhanced magnetization. We may suggest that the anomalous magnetization behavior can be ascribed to frustration in the internal magnetic order for the unirradiated CI particles, and further interparticle interaction for the irradiated CI particles.
Abstract We investigate the magnetic properties in carbonyl iron (CI) particles before and after Ni $$^{+}$$ + and H $$^{+}$$ + ion beam irradiation. Upon increasing temperatures, the saturation magnetization ( $$M_{\text {s}}$$ M s ) in hysteresis loops exhibits an anomalous increase at a high temperature for the unirradiated and the Ni $$^{+}$$ + -beam-irradiated samples, unlike in H $$^{+}$$ + -beam-irradiated sample. Moreover, the magnetization values at low and high temperatures are more intense after Ni $$^{+}$$ + beam irradiation, whereas after H $$^{+}$$ + beam irradiation those are remarkably suppressed. Hematite ( $$\alpha $$ α -Fe $$_{2}$$ 2 O $$_{3}$$ 3 ) phase introduced on the surface of our CI particles undergoes the Morin transition that was observed in our magnetization-temperature curves. The Morin transition causing canted antiferromagnetism above the Morin temperature was found in the unirradiated and Ni $$^{+}$$ + -beam-irradiated samples, but not in H $$^{+}$$ + -beam-irradiated sample. It is thus revealed that the CI particles undergoing the Morin transition cause the anomalous increase in $$M_{\text {s}}$$ M s . We may suggest that Ni $$^{+}$$ + ion beam increases uncompensated surface spins on the CI particles resulting in a more steep Morin transition and the intensified $$M_{\text {s}}$$ M s . Ion-beam irradiation may thus be a good tool for controlling the magnetic properties of CI particles, tailoring our work for future applications.
Flexible and wearable supercapacitor gained considerable attention in recent years due to the demand for flexible energy storage devices in the upcoming wearable electronics appliances. Herein, a highly flexible and wearable planar supercapacitor was fabricated by a simple cut and stick technique over an adhesive tape, utilizing manganese dioxide nanoflowers coated a specially designed carbon fiber cloth (MnO2/CFC) with polyvinyl alcohol/lithium chloride gel polymer electrolyte (PVA/LiCl). The developed MnO2/CFC planar supercapacitor shows a maximum areal capacitance value of similar to 54 mF cm(-2) with excellent energy and power densities (7.5 mu Wh cm(-2) and 2.5 mW cm(-2)). Moreover, the MnO2/CFC planar device exhibited good cyclic stability of similar to 89% and similar to 100% of columbic efficiency for 10000 charge/discharge cycles. And the MnO2/CFC planar supercapacitor considerably retains it areal capacitance even in the bent or rolled state, which demonstrating promising mechanical stability of the device satisfactory for the development of wearable electronic devices.
We have developed a real-time dose monitoring system for a low-energy ion-beam facility. Before we developed the monitoring system, the system had given a substantial error of ±23% when we irradiated an ion beam with a dose as much as 3.0 × 1016 cm−2 on the Si substrate. Moreover, a low irradiation dose as small as 1013 cm−2 was scarcely able to be controlled because of a too short irradiation time of several seconds, producing a greater dose error. To develop a real-time dose monitoring system, in this work, we employed a current integrator in conjunction with a beam stopper, by which a dose of 3.0 ×1016 cm−2 can be exactly irradiated on the sample with less than ±6% error, which was ensured by the measurements of Rutherford backscattering spectroscopy.
Activated carbon, from biomass (pinecone), was synthesized by conventional pyrolysis/chemical activation process and utilized for the fabrication of supercapacitor electrodes. The pinecone‐activated carbon synthesized with 1:4 ratio of KOH (PAC4) showed an increase in surface area and pore density with a considerable amount of oxygen functionalities on the surface. Moreover, PAC4, as supercapacitor electrode, exhibited excellent electrochemical performances with specific capacitance value ∼185 Fg−1 in 1 M H2SO4, which is higher than that of nonactivated pinecone carbon and 1:2 ratio KOH‐based activated carbon (PAC2) (∼144 Fg−1). The systematic studies were performed to design various forms of devices (symmetric and asymmetric) to investigate the effect of device architecture and operating voltage on the performance and stability of the supercapacitors. The symmetric supercapacitor, designed utilizing PAC4 in H2SO4 electrolyte, exhibited a maximum device‐specific capacitance of 43 Fg−1 with comparable specific energy/power and excellent stability (∼96% after 10 000 cycles). Moreover, a symmetric supercapacitor was specially designed using PAC4, as a positive electrode, and PAC2, as a negative electrode, under their electrolytic ion affinity, and which operates in aqueous Na2SO4 electrolyte for a wide cell voltage (1.8 V) and showed excellent supercapacitance performances. Also, a device was assembled with poly(3,4‐ethylene dioxythiophene) (PEDOT) nanostructure, as positive electrode, and PAC4, as a negative electrode, to evaluate the feasibility of designing a hybrid supercapacitor, using polymeric nanostructure, as an electrode material along with biomass‐activated carbon electrode.
H+ irradiation increases the surface hardness of polycarbonate. Nano indentation measurement shows that the hardness increases up to 3.7 GPa at the dose of 5 × 1016 # cm-2 and at the irradiation energy of 150 keV. In addition, the hardness increases with the dose and the energy of H+ irradiation. In accordance with the nano indentation measurement, the Fourier-transform infrared spectroscopy (FTIR) depends on the dose and energy of H+ irradiation. The peak at ∼1500 cm-1 for the aromatic ring and the peak at ∼1770 cm-1 for the C[double bond, length as m-dash]O stretch decrease with increasing dose and energy, while the increase of the dose and energy develops a new C[double bond, length as m-dash]O stretch vibration at ∼1700 cm-1 and forms aromatic hydrocarbons at ∼1600 cm-1. X-ray diffraction experiments are also consistent with the nano indentation measurement and FTIR spectra. Based on the experiments, we discuss a possible mechanism of the surface hardness enhancements by ion beam irradiation.
The post-synthetic annealing (PSA) of metal-organic frameworks (MOFs) are getting more attention in preparing tunable porous materials for energy storage devices. Following this unique strategy, we synthesized and modified the surface texture of the nanostructured zeolite imidazolate framework (ZIF-67) via different annealing temperatures and utilized it as the supercapacitor electrode materials. In particular, the sample at temperature 300 degrees C (ZIF-67@300) achieved a large specific surface area (SSA) similar to 1869 m(2) g(-1) and exhibited a high specific capacity (C-sp) of 339 C g(-1) with better cyclic stability (similar to 94%). Furthermore, a hybrid supercapacitor (HSCs) was assembled using ZIF-67@300 as a positive electrode and oxygen, nitrogen-enriched activated carbon (O, N@AC) as a negative electrode, which operates with a wide cell voltage of 1.5 V. Interestingly, the HSC showed a maximum device-specific capacitance (C-s) of 98 F g(-1) with high specific energy (E) of 30 Wh Kg(-1) and specific power (P) of 28323 W kg(-1), respectively. In addition, the HSCs revealed excellent cyclic stability of similar to 95% for 10,000 continuous galvanostatic charge/discharge (GCD) cycles. Thus, the remarkable electrochemical performance of ZIF-67@300 electrode material as a potential candidate for energy storage devices.
•A developed efficient analytical separation method of two radioisotopes, 67Cu and 67Ga.•The first data for natZn(p,x)67Cu reaction obtained by using the analytical separation method.•The present data being compared with those of the literature and the TENDL-2017 library.