DGA-grafting pyridine for ultra-selective and prior extraction of 99TcO4- from simulated spent nuclear fuel.

Selective and prior extraction of 99TcO4- ahead of uranium and plutonium separation is a beneficial strategy for the modern nuclear fuel cycle. Herein, a novel DGA-grafting pyridine ligand BisDODGA-DAPy (L1) was tailored for the efficient separation of TcO4- from simulated spent nuclear fuel based on the selectivity of pyridine and synergistic effect of diglycolamide (DGA) group. Compared to the ligands BisDOSCA-DAPy (L2) and BisDODGA-MPDA (L3) with similar structure, BisDODGA-DAPy (L1) demonstrated the better separation performance including good extraction efficiency, reusability, and high loading capacity for TcO4- under high acidic medium. The interactions of the ligands with Tc(VII)/Re(VII) have been investigated in detail using FT-IR, 1H NMR titration, UV-Vis spectrophotometric titration, ESI-HRMS and DFT simulations. The extraction mechanism affected by the protonation of ligand was elucidated under different acidity. BisDODGA-DAPy (L1) demonstrated the ultra-selective extraction ability for TcO4- from simulated spent nuclear fuel. The maximum SFTc/U and SFTc/Pu values were up to 1.29 × 104 and 5.08 × 103, respectively. In the presence of 9 × 104-fold excess of NO3-, the extraction of TcO4- was almost unaffected. Moreover, the good radiolytic stability further highlights the promising potential of this ligand for 99Tc separation. DFT calculation revealed the dominant role of DAPy and DODGA in TcO4- extraction, providing the theoretical evidence for BisDODGA-DAPy (L1) to selectively bind TcO4- over NO3-.

Computational Model Based on Optical Coherence Tomography (OCT) Skin Scanning to Identify and Quantify Acute Radiation Dermatitis (ARD): A Prospective Diagnostic Study. / Modelo computacional basado en la tomografía de coherencia óptica (TCO) para identificar y cuantificar la radiodermatitis aguda (RA): estudio observacional prospectivo.

BACKGROUND: Acute radiation dermatitis (ARD) is the most widely reported radiotherapy-induced adverse event. Currently, there is no objective or reliable method to measure ARD. OBJECTIVE: Our main objective was to identify and quantify the effects of radiotherapy with a computational model using optical coherence tomography (OCT) skin scanning. Secondary objectives included determining the ARD impact of different radiotherapeutic schemes and adjuvant topical therapies. METHODS: We conducted a prospective, single-center case series study in a tertiary referral center of patients with breast cancer who were eligible for whole breast radiotherapy (WBRT). RESULTS: A total of 39 women were included and distributed according to the radiotherapeutic schemes (15, 20, and 25 fractions). A computational model was designed to quantitatively analyze OCT findings. After radiotherapy, OCT scanning was more sensitive revealing vascularization changes in 84.6% of the patients (vs 69.2% of the patients with ARD by clinical examination). OCT quantified an increased vascularization at the end of WBRT (P<.05) and a decrease after 3 months (P=.032). Erythematous skin changes by OCT were more pronounced in the 25-fraction regime. CONCLUSION: An OCT computational model allowed for the identification and quantification of vascularization changes on irradiated skin, even in the absence of clinical ARD. This may allow the design of standardized protocols for ARD beyond the skin color of the patients involved.

The TCO concept in German forensic homicide offenders with schizophrenia spectrum disorders - new findings from a file-based, retrospective cross-sectional study.

Introduction: There is evidence that there is a small group of people with schizophrenia spectrum disorders who are more likely to commit homicide than those in the general population. However, there is limited knowledge about the psychopathology that leads to homicide in this group. The aim of this study was to examine two commonly used definitions of the Threat/Control-Override (TCO) concept, which aims to identify a certain risk of serious violence in patients with schizophrenia spectrum disorders. Methods: This is a sub analysis of a file-based, retrospective and exploratory cross-sectional study. All forensic homicide offenders with schizophrenia spectrum disorders who were detained at the Forensic Hospital Berlin as of 31 December 2014 were examined for the occurrence of TCO according to two commonly used definitions. Results: Of a total of 419 forensic patients with schizophrenia spectrum disorders, 78 committed homicide (18.6%). The forensic homicide offenders with schizophrenia spectrum disorders were characterised by being male, unemployed, single and having committed (attempted) manslaughter. Irrespective of the definition used, the entire TCO complex was present in less than a third of the sample. In both definitions, Threat symptoms were slightly less frequent than Control-Override symptoms. While Threat symptoms occurred less frequently in Stompe et al.'s definition, Control-Override symptoms were the most common. With regard to Kröber's definition of Threat and Control-Override, the situation is exactly the opposite. Discussion: Regarding the entire TCO complex, Kröber's definition seems a little more open and Stompe et al.'s more strict (38.5% vs. 35.9%). Since TCO only occurs in about one third of the subjects in both definitions, neither definition appears to be conclusive. A combination with proportions from both definitions could be a contribution to a future definition of TCO. The present study provides scarcely published primary data on psychopathology in homicide offenders with schizophrenia spectrum disorders, especially on the much discussed TCO concept in two definitions. In order to determine the most useful definition of TCO, to avoid false positives and to identify clear psychopathological risk symptoms, larger samples and comparative studies with offenders and non-offenders should be conducted in the future.

Efficient removal of perrhenate/pertechnetate by a pyridinium-based porous polymer.

The extraction of 99TcO4- from radioactive effluents is extremely crucial for the purposes of nuclear disposal and environmental remediation. Herein, utilizing a facile and low-cost synthesis method, we report a pyridinium-based cationic polymer network, CPP-Cl, with impressive adsorption performance and ultrafast adsorption kinetics towards ReO4-. The structure featuring highly density of charged pyridinium units was synthesized, making it an effective adsorbent for capturing ReO4-. The material showed fast ReO4- adsorption kinetics reaching adsorption equilibrium within 30 s, an excellent capture capability of 1069.7 mg/g, and exceptional separation efficiency of 94.3% for removing 1000 ppm ReO4-. Furthermore, it possessed excellent reusability in multiple sorption/desorption trials and good uptake capacity within a widely ranging pH values. It is noteworthy that the extraction efficiency of CPP-Cl for ReO4- from simulated nuclear waste can be up to 94.2%. The favorable performance of the material in multiple tests revealed that CPP-Cl has tremendous potential as a high-efficiency sorbent for capturing 99TcO4-/ReO4- in complex nuclear associated environmental systems.

Titanium Silicide: A Promising Candidate of Recombination Layer for Perovskite/Tunnel Oxide Passivated Contact Silicon Two-Terminal Tandem Solar Cells.

This study proposes a titanium silicide (TiSi2) recombination layer for perovskite/tunnel oxide passivated contact (TOPCon) 2-T tandem solar cells as an alternative to conventional transparent conductive oxide (TCO)-based recombination layers. TiSi2 was formed while TiO2 was made by oxidizing a Ti film deposited on the p+-Si layer. The reaction formation mechanism was proposed based on the diffusion theory supported by experimental results. The optical and electrical properties of the TiSi2 layer were optimized by controlling the initial Ti thicknesses (5-100 nm). With the initial Ti of 50 nm, the lowest reflectance and highly ohmic contact between the TiO2 and p+-Si layers with a contact resistivity of 161.48 mΩ·cm2 were obtained. In contrast, the TCO interlayer shows Schottky behavior with much higher contact resistivities. As the recombination layer of TiSi2 and the electron transport layer of TiO2 are formed simultaneously, the process steps become simpler. Finally, the MAPbI3/TOPCon tandem device yielded an efficiency of 16.23%, marking the first reported efficiency for a device including a silicide-based interlayer.

In vitro and in vivo evaluation of a tetrazine-conjugated poly-L-lysine effector molecule labeled with astatine-211.

BACKGROUND: A significant challenge in cancer therapy lies in eradicating hidden disseminated tumor cells. Within Nuclear Medicine, Targeted Alpha Therapy is a promising approach for cancer treatment tackling disseminated cancer. As tumor size decreases, alpha-particles gain prominence due to their high Linear Energy Transfer (LET) and short path length. Among alpha-particle emitters, 211At stands out with its 7.2 hour half-life and 100% alpha emission decay. However, optimizing the pharmacokinetics of radiopharmaceuticals with short lived radionuclides such as 211At is pivotal, and in this regard, pretargeting is a valuable tool. This method involves priming the tumor with a modified monoclonal antibody capable of binding both the tumor antigen and the radiolabeled carrier, termed the "effector molecule. This smaller, faster-clearing molecule improves efficacy. Utilizing the Diels Alder click reaction between Tetrazine (Tz) and Trans-cyclooctene (TCO), the Tz-substituted effector molecule combines seamlessly with the TCO-modified antibody. This study aims to evaluate the in vivo biodistribution of two Poly-L-Lysine-based effector molecule sizes (10 and 21 kDa), labelled with 211At, and the in vitro binding of the most favorable polymer size, in order to optimize the pretargeted radioimmunotherapy with 211At. RESULTS: In vivo results favor the smaller polymer's biodistribution pattern over the larger one, which accumulates in organs like the liver and spleen. This is especially evident when comparing the biodistribution of the smaller polymer to a directly labelled monoclonal antibody. The smaller variant also shows rapid and efficient binding to SKOV-3 cells preloaded with TCO-modified Trastuzumab in vitro, emphasizing its potential. Both polymer sizes showed equal or better in vivo stability of the astatine-carbon bond compared to a monoclonal antibody labelled with the same prosthetic group. CONCLUSIONS: Overall, the small Poly-L-Lysine-based effector molecule (10 kDa) holds the most promise for future research, exhibiting significantly lower uptake in the kidneys and spleen compared to the larger effector (21 kDa) while maintaining an in vivo stability of the astatine-carbon bond comparable to or better than intact antibodies. A proof of concept in vitro cell study demonstrates rapid reaction between the small astatinated effector and a TCO-labelled antibody, indicating the potential of this novel Poly-L-Lysine-based pretargeting system for further investigation in an in vivo tumor model.

Advancements in Transparent Conductive Oxides for Photoelectrochemical Applications.

Photoelectrochemical cells (PECs) are an important technology for converting solar energy, which has experienced rapid development in recent decades. Transparent conductive oxides (TCOs) are also gaining increasing attention due to their crucial role in PEC reactions. This review comprehensively delves into the significance of TCO materials in PEC devices. Starting from an in-depth analysis of various TCO materials, this review discusses the properties, fabrication techniques, and challenges associated with these TCO materials. Next, we highlight several cost-effective, simple, and environmentally friendly methods, such as element doping, plasma treatment, hot isostatic pressing, and carbon nanotube modification, to enhance the transparency and conductivity of TCO materials. Despite significant progress in the development of TCO materials for PEC applications, we at last point out that the future research should focus on enhancing transparency and conductivity, formulating advanced theories to understand structure-property relationships, and integrating multiple modification strategies to further improve the performance of TCO materials in PEC devices.

Update on cardiac imaging: A critical analysis.

Imaging is instrumental in diagnosing and directing the management of atherosclerosis. In 1958 the first diagnostic coronary angiography (CA) was performed, and since then further development has led to new methods such as coronary CT angiography (CTA), optical coherence tomography (OCT), positron tomography (PET), and intravascular ultrasound (IVUS). Currently, CA remains powerful for visualizing coronary arteries; however, recent studies show the benefits of using other non-invasive techniques. This review identifies optimum imaging techniques for diagnosing and monitoring plaque stability. This becomes even direr now, given the rapidly rising incidence of atherosclerosis in society today. Many acute coronary events, including acute myocardial infarctions and sudden deaths, are attributable to plaque rupture. Although fatal, these events can be preventable. We discuss the factors affecting plaque integrity, such as increased inflammation, medications like statins, and increased lipid content. Some of these precipitating factors are identifiable through imaging. However, we also highlight significant complications arising in some modalities; in CA this can include ventricular arrhythmia and even death. Extending this, we elucidated from the literature that risk can also vary based on the location of arteries and their plaques. Promisingly, there are less invasive methods being trialled for assessing plaque stability, such as Cardiac Magnetic Resonance Imaging (CMR), which is already in use for other cardiac diseases like cardiomyopathies. Therefore, future research focusing on using imaging modalities in conjunction may be sensible, to bridge between the effectiveness of modalities, at the expense of increased complications, and vice versa.

Deposition and Optical Characterization of Sputter Deposited p-Type Delafossite CuGaO2 Thin Films Using Cu2O and Ga2O3 Targets.

CuGaO2 thin films were deposited using the RF magnetron sputtering technique using Cu2O and Ga2O3 targets. The films were deposited at room temperature onto a quartz slide. The sputtering power of Cu2O remained constant at 50 W, while the sputtering power of Ga2O3 was systematically varied from 150 W to 200 W. The films were subsequently subjected to annealing at temperatures of 850 °C and 900 °C in a nitrogen atmosphere for a duration of 5 h. XRD analysis on films deposited with a Ga2O3 sputtering power of 175 W annealed at 900 °C revealed the development of nearly single-phase delafossite CuGaO2 thin films. SEM images of films annealed at 900 °C showed an increasing trend in grain size with a change in sputtering power level. Optical studies performed on the film revealed a transmission of 84.97% and indicated a band gap of approximately 3.27 eV. The film exhibited a refractive index of 2.5 within the wavelength range of 300 to 450 nm.

Computational Model Based on Optical Coherence Tomography (OCT) Skin Scanning to Identify and Quantify Acute Radiation Dermatitis (ARD): A Prospective Diagnostic Study.

BACKGROUND: Acute radiation dermatitis (ARD) is the most widely reported radiotherapy-induced adverse event. Currently, there is no objective or reliable method to measure ARD. OBJECTIVE: Our main objective was to identify and quantify the effects of radiotherapy with a computational model using optical coherence tomography (OCT) skin scanning. Secondary objectives included determining the ARD impact of different radiotherapeutic schemes and adjuvant topical therapies. METHODS: We conducted a prospective, single-center case series study in a tertiary referral center of patients with breast cancer who were eligible for whole breast radiotherapy (WBRT). RESULTS: A total of 39 women were included and distributed according to the radiotherapeutic schemes (15, 20, and 25 fractions). A computational model was designed to quantitatively analyze OCT findings. After radiotherapy, OCT scanning was more sensitive revealing vascularization changes in 84.6% of the patients (vs 69.2% of the patients with ARD by clinical examination). OCT quantified an increased vascularization at the end of WBRT (P<.05) and a decrease after 3 months (P=.032). Erythematous skin changes by OCT were more pronounced in the 25-fraction regime. CONCLUSION: An OCT computational model allowed for the identification and quantification of vascularization changes on irradiated skin, even in the absence of clinical ARD. This may allow the design of standardized protocols for ARD beyond the skin color of the patients involved.

Synthesis and evaluation of fluorine-18 labelled tetrazines as pre-targeting imaging agents for PET.

BACKGROUND: The brain is a challenging target for antibody-based positron emission tomography (immunoPET) imaging due to the restricted access of antibody-based ligands through the blood-brain barrier (BBB). To overcome this physiological obstacle, we have previously developed bispecific antibody ligands that pass through the BBB via receptor-mediated transcytosis. While these radiolabelled ligands have high affinity and specificity, their long residence time in the blood and brain, typical for large molecules, poses another challenge for PET imaging. A viable solution could be a two-step pre-targeting approach which involves the administration of a tagged antibody that accumulates at the target site in the brain and then clears from the blood, followed by administration of a small radiolabelled molecule with fast kinetics. This radiolabelled molecule can couple to the tagged antibody and thereby make the antibody localisation visible by PET imaging. The in vivo linkage can be achieved by using the inverse electron demand Diels-Alder reaction (IEDDA), with trans-cyclooctene (TCO) and tetrazine groups participating as reactants. In this study, two novel 18F-labelled tetrazines were synthesized and evaluated for their potential use as pre-targeting imaging agents, i.e., for their ability to rapidly enter the brain and, if unbound, to be efficiently cleared with minimal background retention. RESULTS: The two compounds, a methyl tetrazine [18F]MeTz and an H-tetrazine [18F]HTz were radiolabelled using a two-step procedure via [18F]F-Py-TFP synthesized on solid support followed by amidation with amine-bearing tetrazines, resulting in radiochemical yields of 24% and 22%, respectively, and a radiochemical purity of > 96%. In vivo PET imaging was performed to assess their suitability for in vivo pre-targeting. Time-activity curves from PET-scans showed [18F]MeTz to be the more pharmacokinetically suitable agent, given its fast and homogenous distribution in the brain and rapid clearance. However, in terms of rection kinetics, H-tetrazines are advantageous, exhibiting faster reaction rates in IEDDA reactions with dienophiles like trans-cyclooctenes, making [18F]HTz potentially more beneficial for pre-targeting applications. CONCLUSION: This study demonstrates a significant potential of [18F]MeTz and [18F]HTz as agents for pre-targeted PET brain imaging due to their efficient brain uptake, swift clearance and appropriate chemical stability.

Synthesis and performance of guanidinium-based cationic organic polymer for the efficient removal of TcO4-/ReO4.

Cationic organic polymers have found relatively extensive utility for TcO4-/ReO4- removal, but the harsh preparation conditions constrain their practical application. The bifunctional guanidinium-based cationic organic polymer (GBCOP) was successfully and facilely synthesized in benign conditions within 1 h. Batch experiments showed that GBCOP exhibited rapid removal kinetics (1 min, >98.0%) and a substantial removal capacity of 536.8 mg/g for ReO4-. Even in 1000-fold co-existing NO3- anions, the removal efficiency of GBCOP for ReO4- was 74.0%, indicating its good selectivity. Moreover, GBCOP had high removal efficiencies for ReO4- across a wide pH (3.0-10.0) range and presented remarkable stability under the conditions of strong acid and base. GBCOP could be reused four times while removing 80.8% ReO4- from simulated Hanford wastewater. SEM and XPS results revealed that the mechanism of ReO4- removal involved Cl- ion exchange within the channels of GBCOP. Theoretical calculation results supported that existing the strong electrostatic interaction between guanidinium and ReO4-. This dual-function GBCOP material is cost-effective and holds significant potential for large-scale preparation, making it a promising solution for TcO4- removal from nuclear wastewater.

Highly Transparent Red Organic Light-Emitting Diodes with AZO/Ag/AZO Multilayer Electrode.

Free-form factor optoelectronics is becoming more important for various applications. Specifically, flexible and transparent optoelectronics offers the potential to be adopted in wearable devices in displays, solar cells, or biomedical applications. However, current transparent electrodes are limited in conductivity and flexibility. This study aims to address these challenges and explore potential solutions. For the next-generation transparent conductive electrode, Al-doped zinc oxide (AZO) and silver (AZO/Ag/AZO) deposited by in-line magnetron sputtering without thermal treatment was investigated, and this transparent electrode was used as a transparent organic light-emitting diode (OLED) anode to maximize the transparency characteristics. The experiment and simulation involved adjusting the thickness of Ag and AZO and OLED structure to enhance the transmittance and device performance. The AZO/Ag/AZO with Ag of 12 nm and AZO of 32 nm thickness achieved the results of the highest figure of merit (FOM) (Φ550 = 4.65 mΩ-1) and lowest roughness. The full structure of transparent OLED (TrOLED) with AZO/Ag/AZO anode and Mg:Ag cathode reached 64.84% transmittance at 550 nm, and 300 cd/m2 at about 4 V. The results demonstrate the feasibility of adopting flexible substrates, such as PET, without the need for thermal treatment. This research provides valuable insights into the development of transparent and flexible electronic devices.

Optimization of radioprotective dose of Juglans nigra leaf extract using response surface methodology.

J. nigra leaf contains mixture of various pharmacologically active compounds and it is assumed that they may have the potential radioprotective effect. The purpose of this work was to predict radioprotective doses by correlating changes in organ distribution of radiopharmaceuticals with extract dose levels and rat body weight using response surface methodology (RSM) based on a second-order polynomial equation. The extract was administered daily by oral gavage to rats at dose of 6.9, 10.3, or 13.7 mg kg-1 body weight (bw) day-1 for 10 days. On the eleventh day, 0.1 ml of the one radiopharmaceutical (Na99mTcO4, 99mTc-dimercaptosuccinic acid and 99mTc-tin colloid) was injected into the tail vein. The statistical parameters: the coefficient of determination (0.81-0.95), the coefficient of variation (3.05-11.1), the adequate precision (8.82-19.12) and the mean relative percentage deviation (± 2.3-8.2) were indicated the precision and reliability of RSM. Using RSM, the predicted daily dose of leaf extract ranging from 11.19 to 11.99 mg kg-1 bw may be considered as an optimal daily radiopotective dose for protection of organs from radiation in cases of planned radiation exposures.

Alkyl modified cationic COFs for preferential trapping of charge dispersed perrhenate: Synergistic hydrophobicity and anion-recognition effects.

Charge dispersed oxoanionic pollutants (such as TcO4- and ReO4-) with low hydrophilicity are typically difficult to be preferentially extracted. Recently, cationic covalent organic frameworks (COFs) have received considerable attention for anions trapping. Two cationic COFs, denoted as Tp-S and Tp-D, were synthesized by incorporating ethyl and cyclic alkylated diquats into 2,2'-bipyridine-based COF. A synergistic effect of hydrophobic channel and anion-recognition sites were achieved by branched chains, which effectively surmounted the Hofmeister bias. Both Tp-S and Tp-D exhibited raising removal performance for surrogate ReO4- at high acidity with adsorption capacities of 435.6 and 291.4 mg g-1, respectively. Obvious variations caused by side chains were displayed in microstructures and adsorption performance. Specially, compared with Tp-D, Tp-S demonstrated desirable priority in uptake capacity and selectivity. In a real-scenario experiment, Tp-S could remove 72.8 % of ReO4- in a simulated Hanford LAW stream, which was attributed to the spatial effects and charge distribution arising from the open and flexible side chains of Tp-S. Otherwise, the rigid cyclic chains endowed pyridine-base Tp-D material an unprecedented alkaline stability. Spectra and theoretical calculations revealed a mechanism of preferential capture based on electrostatic interaction and hydrogen bonding between charge dispersed ReO4-/TcO4- and Tp-S/Tp-D. This work provides an innovative perspective to tailored materials for the treatment of oxoanionic contaminants.

Maculopatía paracentral aguda media y neurorretinopatía macular aguda / Paracentral Acute Middle Maculopathy and Acute Macular Neuroretinopathy

La neurorretinopatía macular aguda es una condición rara con patogenia microvascular. Se presenta con un inicio agudo con escotomas paracentrales correspondientes a lesiones paramaculares evidentes. Los avances en las imágenes multimodales permitieron caracterizar este trastorno de retina y crear nuevos conceptos. Serraf, en el 2013, identificó dos formas por medio de la tomografía de coherencia óptica dominio espectral: el tipo 1 conocido como maculopatía paracentral aguda media en la cual se observa una banda hiperreflectiva en la capa nuclear interna, y el tipo 2 en el cual la banda hiperreflectiva se ubica en la capa nuclear externa, que involucra la zona elipsoide y la zona de interdigitación con el epitelio pigmentario de la retina. Hasta el momento no existe cura; pero se puede actuar sobre los factores de riesgo. Por ser una condición rara y por no existir reportes hasta el momento en Cuba es que se presentan a continuación dos pacientes con cuadros clínicos similares de estas dos variantes; concluyendo la importancia que presentan las imágenes multimodales como medio auxiliar diagnóstico(AU)

Acute macular neuroretinopathy is a rare condition with complex pathogenesis and microvascular cause. It appears with acute onset, with paracentral scotomas corresponding to obvious paramacular lesions. Advances in multimodal imaging made it possible to characterize this retinal disorder and to create new concepts. Serraf, in 2013, identified two forms by spectral domain optical coherence tomography: type 1, known as paracentral acute middle maculopathy, in which a hyperreflective band is observed in the inner nuclear layer; and type 2, in which the hyperreflective band is located in the outer nuclear layer, involving the ellipsoid zone and the zone of interdigitation with the retinal pigment epithelium. Up to this moment, there is no cure; but it is possible to act on the risk factors. Because it is a rare condition and because there are no reports so far in Cuba, two patients with similar clinical pictures of these two variants are presented; concluding the importance of multimodal images as an auxiliary diagnostic tool(AU)

Analysis of Hazy Ga- and Zr-Co-Doped Zinc Oxide Films Prepared with Atmospheric Pressure Plasma Jet Systems.

Co-doped ZnO thin films have attracted much attention in the field of transparent conductive oxides (TCOs) in solar cells, displays, and other transparent electronics. Unlike conventional single-doped ZnO, co-doped ZnO utilizes two different dopant elements, offering enhanced electrical properties and more controllable optical properties, including transmittance and haze; however, most previous studies focused on the electrical properties, with less attention paid to obtaining high haze using co-doping. Here, we prepare high-haze Ga- and Zr-co-doped ZnO (GZO:Zr or ZGZO) using atmospheric pressure plasma jet (APPJ) systems. We conduct a detailed analysis to examine the interplay between Zr concentrations and film properties. UV-Vis spectroscopy shows a remarkable haze factor increase of 7.19% to 34.8% (+384%) for the films prepared with 2 at% Zr and 8 at% Ga precursor concentrations. EDS analysis reveals Zr accumulation on larger and smaller particles, while SIMS links particle abundance to impurity uptake and altered electrical properties. XPS identifies Zr mainly as ZrO2 because of lattice stress from Zr doping, forming clusters at lattice boundaries and corroborating the SEM findings. Our work presents a new way to fabricate Ga- and Zr-co-doped ZnO for applications that require low electrical resistivity, high visible transparency, and high haze.

Neutral MOF Anion Receptor: Radical-Promoted Precise Anion Recognition.

Precise ion recognition plays a key role in the anionic decontamination in water. However, the established anionic recognition based on neutral or cationic anion receptor is still restricted by the inherent limitation, such as narrow application scope in organic solvent rather than water for neutral anion receptor and poor selectivity due to non-directional electrostatic interaction for cationic anion receptor. Herein, for the first time, a neutral metal-organic framework (MOF) anion receptor is shown, enabling precise anion recognition, for example, the presence of a variety of 1000-fold competitive anions does not affect the selective adsorption of the target anion at all. A radical-dominating anion-recognition mechanism is proposed for rationalizing the efficacy of the neutral MOF.

CTAB assisted evaporation-induced self-assembly to construct imidazolium-based hierarchical porous covalent organic polymers for ReO4-/TcO4- removal.

Evaporation-induced self-assembly method (EISA) was a facile and reliable method to synthesize porous materials. Herein, we report a kind of hierarchical porous ionic liquid covalent organic polymers (HPnDNH2) under cetyltrimethylammonium bromide (CTAB) assisted by EISA for ReO4-/TcO4- removal. Unlike covalent organic frameworks (COFs), which usually needed to be prepared in a closed environment or with a long reaction time, HPnDNH2 in this study was prepared within 1 h in an open environment. It was worth noting that CTAB not only served as a soft template for forming pore, but also induced ordered structure, which was verified by SEM, TEM, and Gas sorption. Benefit from its hierarchical pore structure, HPnDNH2 exhibited higher adsorption capacity (690.0 mg g-1 for HP1DNH2 and 808.7 mg g-1 for HP1.5DNH2) and faster kinetics for ReO4-/TcO4- than 1DNH2 (without employing CTAB). Additionally, the material used to remove TcO4- from alkaline nuclear waste was seldom reported, because combining features of alkali resistance and high uptake selectivity was not easy to achieve. In this study, in the case of HP1DNH2, it displayed outstanding adsorption efficiency toward aqueous ReO4-/TcO4- in 1 mol L-1 NaOH solution (92%) and simulated Savannah River Site High-level waste (SRS HLW) melter recycle stream (98%), which could be a potentially excellent nuclear waste adsorbing material.

Ultra-stable 3D pyridinium salt-based polymeric network nanotrap for selective 99TcO4-/ReO4- capture via hydrophobic and steric engineering.

Selective capture of radioactive 99TcO4- from highly alkaline nuclear waste is highly desirable for environmental remediation and waste disposal. However, the combined features of adsorbents with excellent chemical stability and high capture selectivity for 99TcO4- have not yet been achieved. Herein, we report an ultra-stable 3D pyridinium salt-based polymeric network (TMP-TBPM) nanotrap with remarkable radiation, acid and base stability for selective capture of ReO4- via hydrophobic engineering and steric hindrance, a non-radioactive surrogate of 99TcO4-. The batch capture experiments show that TMP-TBPM has high capture capacity (918.7 mg g-1) and fast sorption kinetics (94.3 % removal in 2 min), which can be attributed to the high density of pyridinium salt-based units on the highly accessible pore channels of 3D interconnected low-density skeleton. In addition, the introduction of abundant alkyl and tetraphenylmethane units into the 3D framework not only greatly enhanced the hydrophobicity and stability of TMP-TBPM, but also significantly improved the affinity toward 99TcO4-/ReO4-, enabling reversible and selective capture of 99TcO4-/ReO4- even under highly alkaline conditions. This study exhibits the great potential of 3D pyridinium salt-based polymeric network nanotrap for 99TcO4-/ReO4- capture from highly alkaline nuclear waste, providing a new strategy to construct high-performance cationic polymeric sorbents for radioactive wastewater treatment.