bluuebunny/crossref_metadata_2025 huggingface dataset:
Amino Acids for Perovskite Light‐Emitting Diodes: Conformations, Mechanisms, and Applications
Authors: Islam Amjad , Haider Zeeshan , Imran Muhammad , Li Ming‐De , Hassan Rizwan Ul
Published: October 2024

Among the most auspicious and efficient surface ligand candidates or additives to raise the efficiency of perovskite light‐emitting diodes (PeLEDs) are amino acids (AAs), possessing a combination of amino group and carboxylic group. The AA molecules exhibit significant promise for coherent tailoring their molecular conformations to yield remarkable advantages and multi‐functional properties. This raises a question that how PeLED devices can benefit greatly from the small amount of AA molecules integrated in perovskite films. In order to set up a structure–property relationship, the mysteries of the extraordinary improvement in performance of PeLEDs through AAs modification are disclosed. Furthermore, there is a critical discussion of workable guidelines for exploring AAs with optimal molecular conformations. Moreover, recent developments in blue, green, and red PeLED devices incorporating AAs are also highlighted in detail. Lastly, suggestions for future directions in research as well as the logical construction of functional AA molecules for potent and more stable PeLED devices are presented.
New Horizons for Temperature Sensing and Bioimaging Using Er3+‐Doped Core@Shell Nanoparticles and Effects of H2O and D2O Solvents on Their Spectroscopic Properties
Authors: Ryszczyńska Sylwia , Soler‐Carracedo Kevin , Ekner‐Grzyb Anna , Jurga Natalia , Ćwierzona Maciej , Piątkowski Dawid , Grzyb Tomasz
Published: October 2024

Lanthanide‐doped nanoparticles (NPs) exhibit temperature‐dependent luminescence, enabling the design of luminescent nanothermometers for industrial and medical applications. This research demonstrates the temperature‐sensing properties of NaYF4:7.5%Er3+@NaYF4 and NaErF4@NaYF4 NPs, which have a hexagonal shape and average size of 17 nm. Their core@shell structure is confirmed using high‐resolution transmission electron microscopy, and they exhibit intense upconversion (UC) emission under 1532 nm excitation in H2O and D2O colloids. The recorded spectra show Er3+ emission bands with varying intensity ratios depending on the Er3+ concentration, chosen solvent, and temperature. The spectroscopic properties of the studied NPs allow for their excitation and observation of emission within biological windows, which makes them useful for bio‐related applications. The emission of prepared NPs is analyzed as a function of temperature from 298 up to 358/363 K in H2O and D2O. The ratios for thermally‐coupled levels  and non‐TCLs and their relative sensitivities are studied. For the high dopant concentration sample in water, the O─H vibrations and blue shift in the absorption spectrum lead to a record relative sensitivity of 2.50% K−1 (at 363 K) for the 2H11/2/4I11/2 ratio. The use of synthesized NPs for bioimaging under 1550 nm excitation is also demonstrated to observe their accumulation in the guts of Daphnia magna.
Processable Circularly Polarized Luminescence for the Synthesis of Chiral Plasmonic Nanoparticles
Authors: Wang Zhiyu , Li Anran , Cao Qinxuan , Liang Wenfei , Feng Jianning , Chang Kin Ting , Xu Zewei , Srivastava Abhishek K , Lu Haipeng
Published: October 2024

Circularly polarized light is previously shown as a chiral bias to enable the synthesis of chiral plasmonic nanomaterials through light‐matter interactions. The traditional approach for circularly polarized light generation relies on a “top‐down” approach by removing undesired light polarization through optics, which suffers from energy loss and compatibility issues. An alternative approach is to develop chiral phosphors that emit efficient circularly polarized luminescence (CPL). However, most materials fail to produce processable CPL with both high quantum yield and dissymmetry factors, let alone the synthesis of chiral nanomaterials. Herein, a liquid‐crystal‐templated framework is developed to assemble halide perovskite nanocrystals, CsPbX3 (X = Cl, Br, I), and achieved efficient CPL with the record‐high figure of merit (FM) for three primary colors (Red, Green, Blue). The fidelity of the CPL is further demonstrated in the synthesis of chiral gold nanoparticles, where a five‐fold increase in optical activity is achieved.
Vertical Hierarchical Architecture of Niobium Diselenide Nanosheets Loaded ZnO Nanorods for High‐Performance Self‐Powered Broadband Photodetection
Authors: Kumar Mahesh , Huang Bohr‐Ran , Saravanan Adhimoorthy , Chen Sheng‐Chi , Hsiao Wesley Wei‐Wen , Sun Hui
Published: October 2024

Materials with low‐dimensional (1D–2D) structures hold significant promise for electronic and optoelectronic applications owing to their distinctive structural features and inherent properties. These characteristics render them of substantial interest across various scientific domains, particularly in applications related to energy storage, such as supercapacitors and lithium‐ion batteries. Due to their high surface‐to‐volume ratios and unique geometric properties, low‐dimensional materials have attracted considerable attention in developing advanced broadband photodetectors (PDs) with enhanced performance capabilities. In this study, for the first time, the study reports self‐powered broadband PDs based on vertical‐core‐shell niobium diselenide (NbSe2)‐ZnO nanorods (ZNRs), which are produced using a hydrothermal method. Remarkably, the NbSe2(3 ml) doped ZNRs‐based device exhibits outstanding responsivity of 0.62, 23.21, 5.35, 1.11, 0.30 AW−1, detectivity of 2.15 × 1010, 4.10 × 1011, 1.62 × 1011, 8.83 × 1010, 1.42 × 1011 Jones, and high sensitivity of 8.74 × 104%, 5.78 × 105%, 2.71 × 105%, 2.79 × 105%, 1.43 × 105% at wavelengths of 365, 456, 532, 632, and 850 nm, respectively, at zero bias. The NbSe2(3ml)‐ZNRs device showed a rapid response and fall times of 37 ms and 40 ms, enabled by NbSe2 superconductivity. The concept introduced in this study is strongly believed to possess significant potential and can be extensively applied in developing next‐generation integrated optoelectronic, clean energy technology, and photodetection devices based on 1D/2D nanostructures.
Multi‐Channel Optical Encryption Film With Strong Circularly Polarized Luminescence and High Quantum Yield
Authors: Jia Shengzhe , Yang Bingbing , Zhang Yongsheng , Du Jing , Tao Tiantian , Tang Jiaxuan , Zhang Jiayin , Liao Peng , Tang Weiwei , Gong Junbo
Published: October 2024

Developing a sustainable security module with multiple optical states is important to deter counterfeits, but is challenging. This work designs a kind of chiral luminescent film through the co‐assembly of the CNCs and d‐glucose, simultaneously doped with the lanthanide complex and organic dye. Superior mechanical performance makes it undertake various deformations, including twist, and tension without breaking. Meanwhile, this film has unique optical characteristics. On the one hand, the chiroptical signals can be manipulated through the matching of the photonic bandgap and fluorescence peak. On the other hand, due to the co‐assembly with two luminophores, the film displays the excitation wavelength (Ex)‐dependent circularly polarized luminescence properties. Under the Ex of 275 nm, the film simultaneously integrates a large dissymmetry factor of −0.3898, a high quantum yield of 69.19%, and a considerable lifetime of 1381 µs, which has exceeded most reported chiral luminescent assemblies. These multimodal and convertible optics endow the film with practical applications in the anti‐counterfeit. It can be designed as a security label or used as a written paper to encrypt the information. Even in humid surroundings, this security effect is still ensured.
Unsupported Nanoporous Copper Catalyzed Insertion of Carbenes from α‐Diazo Compounds into Hydrosilanes
Authors: Jiang Ruyi , Zheng Xiaojun , Wang Cuiping , Wei Wanguo , Jin Tienan , Zhao Yuhui , Zhang Zhiqiang
Published: October 2024

The insertion of diazo carbene into Si−H bonds with unsupported nanoporous copper (CuNPore) catalyst has been developed. α‐Aryl diazoesters, diazophosphonates, and unstable aryl diazoalkyls can be used as carbene precursors to exquisitely insert into the Si−H bond of silanes. A variety of α‐silylesters, silylphosphonate, and functionalized arylsilane were obtained in 35–82% yields. The reusability feature of the CuNPore catalyst for this insertion reaction demonstrated its high heterogeneous catalytic activity and practicality. Further, mechanistic studies revealed that the insertion of carbene from diazo compounds into the Si−H bond may include a three‐center concerted transition state on CuNPore.
Leveraging Blood Components for 3D Printing Applications Through Programmable Ink Engineering Approaches
Authors: Sobreiro‐Almeida Rita , Santos Sara C. , Decarli Monize C. , Costa Marcelo , Correia Tiago R. , Babilotte Joanna , Custódio Catarina A. , Moroni Lorenzo , Mano João F.
Published: October 2024

This study proposes a tunable ink engineering methodology to allow 3D printing processability of highly bioactive but otherwise low‐viscous and unprintable blood‐derived materials. The hypothesis relies on improving the viscoelasticity and shear thinning behavior of platelet lysates (PL) and albumins (BSA) solutions by covalent coupling, enabling simultaneous extrusion and photocrosslinking upon filament deposition. The available amine groups on proteins (PL and BSA) are exploited for coupling with carboxyl groups present in methacrylated proteins (hPLMA and BSAMA), by leveraging carbodiimide chemistry. This reaction enabled the creation of a pre‐gel from these extremely low‐viscous materials (≈ 1 Pa), with precise tuning of the reaction, resulting in inks with a range of controlled viscosities and elasticities. Shape‐fidelity analysis is performed on 3D‐printed multilayered constructs, demonstrating the ability to reach clinically relevant sizes (>2 cm in size). After photocrosslinking, the scaffolds showcased a mechanically robust structure with sustained protein release over time. Bioactivity is evaluated using human adipose‐derived stem cells, resulting in increased viability and metabolic activity over time. The herein described research methodology widens the possibilities for the use of low‐viscosity materials in 3D printing but also enables the direct application of patient and blood‐derived materials in precision medicine.
Copper Paste Printed Paper‐Based Dual‐Band Antenna for Wearable Wireless Electronics
Authors: Yang Wendong , Zhao Xun , Nan Jingchang , Hengge Michael , List‐Kratochvil Emil J. W.
Published: October 2024

Wearable wireless electronics is becoming a significant research area because of the unique features of this technology. Within this field printed antennas are the key electrical component accomplishing the signal transmission and energy harvesting tasks and at the same these antennas need to be lightweight, environmentally friendly, safe to wear, and easy to conform. Currently, the majority of available paper‐based antennas are designed for RFID, sensing, UWB, WLAN, and medical applications, with just a few being utilized in wearable applications, particularly for wireless body area network (WBAN). Furthermore, few studies have been conducted on the usage of printable copper conductive materials and low‐temperature plasma technique for the fabrication of such antennas. This study demonstrates the realization of a dual‐band paper‐based wearable antenna by screen‐printing of a plasma‐sintered conductive copper paste. The copper paste, composed of 51 wt% solid particles, can easily produce desired conductive patterns on photo paper after printing and a subsequent plasma sintering, with a good adhesion. The antenna designed on photopaper operates in the frequency bands of 1.73–2.55 GHz and 7.66–8.89 GHz. Free‐space simulation and measurement results reveal that the antenna exhibits stable radiation performance in the targeted WBAN (2.4–2.4835 GHz) and X uplink (7.9–8.4 GHz) frequency bands, together with low profile, excellent conformality and acceptable SAR values on the body and no electronic waste formed after disposal, making it a competitive candidate for usage in wearable wireless electronics.
Metal‐Organic Framework Hosted Silicon for Long‐Cycling, Low‐Cost, and Flexible Batteries
Authors: Phiri Isheunesu , Kim Jeong‐Tae , Kennedy Ssendagire , Ryou Sun‐Yul
Published: October 2024

Developing biodegradable electrodes is a significant step toward environmental sustainability and cost reduction in battery technology. This paper presents a new approach that utilizes metal‐organic framework (MOF)‐encapsulated silicon nanoparticles (SiNPs) as the active anode material within a cellulose‐based electrode. The electrode is free‐standing, flexible, biodegradable, and significantly reduces the strain experienced by SiNPs during volume expansion, resulting in improved capacity and cycle life stability of SiNPs. The high porosity of the electrode creates efficient lithium (Li+) ion transport channels and enhances electrolyte absorption, thus promoting effective contact between the electrolyte and active material. The outcome is rapid electrode kinetics and a highly reversible discharge capacity of 1744.6 mAh g−1 at 0.5 A g−1 versus Li/Li+ over 1000 cycles. Further, full cell tests are conducted that demonstrate a stable cycle performance exceeding 3400 cycles, with an initial discharge capacity retention of 80.5% at 0.5 A g−1. By employing cellulose and avoiding toxic organic solvents and binders, the proposed approach is promising for a substantial reduction of the production costs of Li‐ion batteries. The scalability of the proposed method further enhances its practical viability, offering intriguing economic implications for the future of battery technology.
Simultaneous achieving color‐tuning long persistent luminescence and phosphorescent quantum yield of 81.05% in 2D organic metal halide perovskite
Authors: Wang Zheng , Li Chen‐Qi , Mo Jun‐Ting , Pan Mei
Published: October 2024

Ionically bonded organic metal halide perovskite‐like luminescent materials, which incorporate organic cations and metal halides, have emerged as a versatile multicomponent material system. However, these materials still face challenges in terms of low phosphorescence quantum yields and limited long persistent luminescence (LPL) colors. Herein, we present the design and synthesis of an intraligand charge‐transfer organic‐based metal halide perovskite‐like material, in which organic cations form a compact supramolecular hydrogen‐bonded organic framework (HOF) structure, exhibiting crystallization‐induced phosphorescence emission of ligand, while metal halides form a unique two‐dimensional (2D) structure that displays intrinsic self‐trapped excitons (STE) emission under the radiation of UV light. Notably, the metal halide hybrid is found to exhibit enhanced phosphorescent photoluminescence efficiency of up to 81.05% and tunable LPL from cyan to orange compared to the pristine organic phosphor, due to the structural distortion and scaffolding effects of 2D metal halides as well as a well‐packed HOF structure. Optical characterizations and theoretical calculations reveal that charge transfer from organic cations and halogen to ligand as well as STE from inorganic layers are responsible for the tunable LPL. Meanwhile, the high‐efficiency phosphorescent quantum yield is attributed to stronger hydrogen bond stacking as well as structural distortion of metal halogen bands. Thus, the obtained LPL provides potentials in anti‐counterfeiting, security systems, and so on.
Where did they come from, where did they go? Niche conservatism in woody and herbaceous plants and implications for plant‐based paleoclimatic reconstructions
Authors: Quirk Zack J. , Smith Selena Y. , Paul Acosta R. , Poulsen Christopher J.
Published: October 2024

Premise

The ecological conditions that constrain plants to an environmental niche are assumed to be constant through time. While the fossil record has been used previously to test for niche conservatism of woody flowering plants, additional studies are needed in other plant groups especially since they can provide insight with paleoclimatic reconstructions, high biodiversity in modern terrestrial ecosystems, and significant contributions to agriculture.

Methods

We tested climatic niche conservatism across time by characterizing the climatic niches of living herbaceous ginger plants (Zingiberaceae) and woody dawn redwood (Metasequoia) against paleoniches reconstructed based on fossil distribution data and paleoclimatic models.

Results

Despite few fossil Zingiberaceae occurrences in the latitudinal tropics, unlike living Zingiberaceae, extinct Zingiberaceae likely experienced paratropical conditions in the higher latitudes, especially in the Cretaceous and Paleogene. The living and fossil distributions of Metasequoia largely remain in the upper latitudes of the northern hemisphere. The Zingiberaceae shifted from an initial subtropical climatic paleoniche in the Cretaceous, toward a temperate regime in the late Cenozoic; Metasequoia occupied a more consistent climatic niche over the same time intervals.

Conclusions

Because of the inconsistent climatic niches of Zingiberaceae over geologic time, we are less confident of using them for taxonomic‐based paleoclimatic reconstruction methods like nearest living relative, which assume a consistent climatic niche between extant and extinct relatives; we argue that the consistent climatic niche of Metasequoia is more appropriate for these reconstructions. Niche conservatism cannot be assumed between extant and extinct plants and should be tested further in groups used for paleoclimatic reconstructions.
Functional disabilities and adverse well‐being by COVID‐19 and Long COVID history and employment status: 2022 Behavioral Risk Factor Surveillance System
Authors: Silver Sharon R. , Li Jia , Ford Nicole D. , Saydah Sharon H.
Published: October 2024

Background

Long COVID can lead to functional disabilities and decreased well‐being and limit the ability to work. No study has yet assessed associations of SARS‐CoV‐2‐infection and Long COVID with specific measures of well‐being and functional disabilities among workers by employment status.

Methods

Using data from the U.S. Behavioral Risk Factor Surveillance System, we assessed the prevalence of functional disabilities and well‐being measures among adults of prime working age (25–54 years) by employment status and self‐reported COVID‐19 and Long COVID history. Within each employment status, we generated adjusted prevalence ratios (aPRs) comparing respondents from each 2022 COVID‐19/Long COVID category to respondents in that employment status before the pandemic (2019).

Results

In 2022, prevalences of each functional disability except vision and all adverse well‐being measures were highest among the 9.2% of respondents reporting a history of Long COVID. For each outcome, prevalences were lowest for workers and highest among those unable to work. 2022 prevalence of cognitive disability (16.4% of employees, 21.4% of the self‐employed) and depression (31.2% and 36.4%, respectively) among workers reporting a history of Long COVID were more than double 2019 levels. Increases in cognitive disability and depression were lower but statistically significant among workers not reporting a history of Long COVID.

Conclusions

The high prevalence of functional disabilities and adverse well‐being among workers reporting a history of Long COVID have implications for workers and employers. Also concerning are smaller increases among workers not reporting a history of Long COVID, given the large number of affected workers. Mitigating the effects of Long COVID on workers will involve efforts in multiple domains: reducing incidence, increasing healthcare practitioner awareness, improving diagnosis and treatments, and increasing employer awareness of best practices for accommodating workers with Long COVID.
Synaptic and extrasynaptic distribution of NMDA receptors in the cortex of Alzheimer's disease patients
Authors: Escamilla Sergio , Badillos Raquel , Comella Joan X. , Solé Montse , Pérez‐Otaño Isabel , Mut Jose V. Sánchez , Sáez‐Valero Javier , Cuchillo‐Ibáñez Inmaculada
Published: October 2024

BACKGROUND

Synaptic and extrasynaptic distribution of N‐methyl‐D‐aspartate receptors (NMDARs) has not been addressed in the brain from Alzheimer´s disease (AD) subjects, despite their contribution to neurodegeneration.

METHODS

We have developed a protocol to isolate synaptic and extrasynaptic membranes from controls and AD frontal cortex. We characterized the distribution of the NMDAR subunits GluN2B, GluN2A, GluN1, and GluN3A, as well as post‐translational modifications, such as phosphorylation and glycosylation.

RESULTS

Lower levels of synaptic GluN2B and GluN2A were found in AD fractions, while extrasynaptic GluN2B and GluN1 levels were significantly higher; GluN3A distribution remained unaffected in AD. We also identified different glycoforms of GluN2B and GluN2A in extrasynaptic membranes. Synaptic Tyr1472 GluN2B phosphorylation was significantly lower in AD fractions.

DISCUSSION

Reduction of synaptic NMDAR subunits, particularly for GluN2B, is likely to contribute to synaptic transmission failure in AD. Additionally, the increment of extrasynaptic NMDAR subunits could favor the activation of excitotoxicity in AD.

Highlights

New protocol to isolate synaptic and extrasynaptic membranes from the human cortex.

Low GluN2B and GluN2A levels in Alzheimer´s disease (AD) synaptic membranes.

High GluN2B and GluN1 levels in AD extrasynaptic membranes.

Specific glycoforms of extrasynaptic GluN2B and GluN2A.

Low phosphorylation at Tyr1472 in synaptic GluN2B in AD.
Stable and Recyclable Copper Nanoclusters with Exposed Active Sites for Broad‐Scope Protosilylation in Open Air
Authors: Wen Songwei , Zhang Chengkai , Liu Li‐Juan , Wang Zhi , Sun Di , He Jian
Published: October 2024

Despite recent advances in cluster‐based catalysis for organic synthesis, the substrate scope of reactions catalyzed by metal nanoclusters is typically not superior to previously established catalytic systems. Herein, we develop new atomically precise copper nanoclusters for protosilylation, with scope expanding to alkenes and simple enynes that were not suitable for prior synthetic methodologies with traditional copper complexes. The involvement of a second copper center in the metal kernel during the migratory insertion step is thought to be responsible for the expanded scope. In addition, the reaction is highly compatible with water and can be carried out in open air rather than under inert gas protection. Mechanistic studies suggest that the cluster‐catalyzed protosilylation proceeds in the absence of silyl radicals. The current findings demonstrate the potential of using metal nanoclusters for practical and sustainable chemical synthesis.
Novel Inorganic‐Organic Dual‐Photosensitizing Dinuclear‐Metal Self‐Assembly System for Efficient Artificial Photosynthesis without Sacrificial Electron Donors
Authors: Wang Jiaxin , Song Tianqun , Liu Zheyuan , Yun Qinbai , Sun Juehan , Zhang Ying , Yuan Kuo , Zhong Dichang , Tang Zhiyong , Lu Tongbu
Published: October 2024

Owing to the unique synergistic effect, dinuclear‐metal‐molecule‐catalysts (DMCs) show excellent performance in catalytic fields. However, for overall photocatalytic CO2 reaction (CO2RR), it is still a challenge to construct well‐matched photosensitizer (PS) components for DMCs‐based photocatalysts. Inorganic‐quantum‐dot PS possesses capacities of multiple exciton generation and catalyzing water oxidation but is incompatible with DMCs. In contrast, organic PS can be covalently linked with DMCs but inescapable of using sacrificial electron donors. For overall photocatalytic CO2RR, organic–inorganic dual‐photosensitizing system might be a promising candidate. Herein, we employed covalent‐linking and electrostatic‐driven approaches to construct the self‐assembly of pyrene‐sensitized Co2L DMCs (Py‐Co2L) and perovskite (PVK) quantum dots, i.e., PVK@[Py‐Co2L]. Using H2O as an electron donor, PVK@[Py‐Co2L] realized 105.24 μmol ⋅ g−1⋅h−1 CO yield in photocatalytic CO2RR, much higher than PVK (15.44 μmol ⋅ g−1⋅h−1) and PVK@Co2L (32.30 μmol ⋅ g−1 ⋅ h−1), ascribing to the efficient photogenerated charge separation and transfer. The experimental results and theoretical investigations demonstrated that the pyrene linked on Co2L boosted the electron delivery from PVK to DMCs. Besides, this strategy could also be extended to the photocatalytic H2 evolution coupled with alcohol oxidation. As a proof‐of‐concept, our work lightens the integration of DMCs, organic and inorganic PS components, promoting the development of photocatalysis without sacrificial electron donors.
Engineering a Cu‐Pd Paddle‐Wheel Metal–Organic Framework for Selective CO2 Electroreduction
Authors: Zhang Ruirui , Liu Yan , Ding Pan , Huang Juanjuan , Dierolf Martin , Kelly Shelly D. , Qiu Xinqi , Chen Yishuo , Hussain Mian Zahid , Li Weijin , Bunzen Hana , Achterhold Klaus , Pfeiffer Franz , Sharp Ian D. , Warnan Julien , Fischer Roland A.
Published: October 2024

Optimizing the binding energy between the intermediate and the active site is a key factor for tuning catalytic product selectivity and activity in the electrochemical carbon dioxide reduction reaction. Copper active sites are known to reduce CO2 to hydrocarbons and oxygenates, but suffer from poor product selectivity due to the moderate binding energies of several of the reaction intermediates. Here, we report an ion exchange strategy to construct Cu−Pd paddle wheel dimers within Cu‐based metal–organic frameworks (MOFs), [Cu3‐xPdx(BTC)2] (BTC=benzentricarboxylate), without altering the overall MOF structural properties. Compared to the pristine Cu MOF ([Cu3(BTC)2], HKUST‐1), the Cu−Pd MOF shifts CO2 electroreduction products from diverse chemical species to selective CO generation. In situ X‐ray absorption fine structure analysis of the catalyst oxidation state and local geometry, combined with theoretical calculations, reveal that the incorporation of Pd within the Cu−Pd paddle wheel node structure of the MOF promotes adsorption of the key intermediate COOH* at the Cu site. This permits CO‐selective catalytic mechanisms and thus advances our understanding of the interplay between structure and activity toward electrochemical CO2 reduction using molecular catalysts.
Atomically Asymmetrical Ir−O–Co Sites Enable Efficient Chloride‐Mediated Ethylene Electrooxidation in Neutral Seawater
Authors: Cai Linke , Liu Yao , Gao Ying , Zhao Bo‐Hang , Guan Jiacheng , Liu Xiao , Zhang Bin , Huang Yi
Published: October 2024

The chloride‐mediated ethylene oxidation reaction (EOR) of ethylene chlorohydrin (ECH) via electrocatalysis is practically attractive because of its sustainability and mild reaction conditions. However, the chlorine oxidation reaction (COR), which is essential for the above process, is commonly catalyzed by dimensionally stable anodes (DSAs) with high contents of precious Ru and/or Ir. The development of highly efficient COR electrocatalysts composed of nonprecious metals or decreased amounts of precious metals is highly desirable. Herein, we report a modified Co3O4 with a single‐atom Ir substitution (Ir1/Co3O4) as a highly efficient COR electrocatalyst for chloride‐mediated EOR to ECH in neutral seawater. Ir1/Co3O4 achieves a Faradaic efficiency (FE) of up to 94.8 % for ECH generation and remarkable stability. Combining experimental results and density functional theory (DFT) calculations, the unique atomically asymmetrical Ir−O−Co configuration with a strong electron coupling effect in Ir1/Co3O4 can accelerate electron transfer to increase the reaction kinetics and maintain the structural stability of Co3O4 during COR. Moreover, a coupling reaction system integrating the anodic chloride‐mediated and cathodic H2O2‐mediated EOR show a total FE of ~170 % for paired electrosynthesis of ECH and ethylene glycol (EG) using ethylene as the raw material. The technoeconomic analysis highlights the promising application prospects of this system.
Oligonucleotide therapeutics in sports? An antidoping perspective
Authors: Parr Maria K. , Keiler Annekathrin M.
Published: October 2024

Within the last two decades, the European Medicines Agency and the US Food and Drug Administration have approved several gene therapies. One category is oligonucleotide therapeutics, which allow for the regulation of the expression of target genes. Besides already approved therapeutics, there are several preclinical and clinical trials ongoing. The World Anti‐Doping Agency prohibits the use of “nucleic acids or nucleic acid analogs that may alter genome sequences and/or alter gene expression by any mechanism” as a nonspecified method at all times. Hence, the administration of nucleic acids or analogs by athletes would cause an Anti‐Doping Rule Violation. Herein, we discuss types of oligonucleotide therapeutics, their potential to be misused in sports, and considerations to sample preparation and mass spectrometric approaches with regard to antidoping analysis.
Beyond one size fits all: Probing patient choices in gestational diabetes management, from screening to postpartum
Authors: Mobin Ayman , Obeid Amir , El‐Kebbi Imad , Everett Dean , Ibrahim Saleh , Farhat Joviana , Al‐Omari Basem
Published: October 2024

During antenatal care, gestational diabetes mellitus (GDM) screening is crucial for early diagnosis and treatment to ameliorate clinical outcomes and limit health care expenses. Dietary management and physical activity are central to GDM treatment, however, adherence is often influenced by personal preferences, socioeconomic barriers, and psychological stress. Pharmacologically, insulin and oral hypoglycemic medications, are the main GDM treatment that can be subject to patients' resistance due to fears of needles and side effects. Metformin is increasingly preferred for its ease of administration and lower cost. In the postpartum stage, regular screening for type 2 diabetes mellitus (T2DM) should always be considered despite the possible limitations that could arise, including communication gaps, lack of long‐term focus, and personal barriers. Overall, women with GDM prefer personalized, flexible management plans that consider their lifestyle, support from health care professionals (HCPs), and family involvement. Addressing psychological and socioeconomic barriers through education, counseling, and support networks is crucial for improving adherence and health outcomes. Enhancing patient‐centered care and shared decision‐making can empower women with GDM to manage their condition effectively and maintain lifestyle changes postpartum. Therefore, this review aimed to assess pregnant women's preferences in GDM management, focusing on screening, dietary recommendations, physical activity, and treatment. Additionally, this review examined GDM care in terms of these patients' quality of life and postpartum experiences.
On the Properties of PLS for Analyzing Two‐Level Factorial Experimental Designs
Authors: Borràs‐Ferrís Joan , Folch‐Fortuny Abel , Ferrer Alberto
Published: October 2024

We present here a novel methodology to analyze data from two‐level factorial experimental designs, with or without missing runs, with just one method: partial least squares regression with one response variable (PLS1, hereinafter PLS). This property is very attractive for practitioners because, to the best of our knowledge, no other statistical tool has comparable versatility. In the case of a full and fractional factorial design, the one‐PLS component model yields the same analytical solution as multiple linear regression (MLR), not only in the estimation of the effects but also in their statistical significance. When having missing runs in the factorial design, PLS is of particular interest as it is a powerful tool when dealing with complex correlation structures, as opposed to MLR. Thus, we challenge the widely held view that PLS is useful only when dealing with nonexperimental design (i.e., correlated observational data). The methodology is illustrated by two illustrative examples and synthesized by an easy‐to‐follow route map useful for practitioners.
Enrichment Strategies for Low‐Abundant Single Nucleotide Mutations
Authors: Guo Chen , Ding Ruolin , Zhao Zhihe , Guo Jian , Li Feng
Published: October 2024

Over the past three decades, significant advancements have been made in mutation enrichment methods, driven by the increasing need for precise and efficient identification of rare genetic variants associated with diseases. Mutation‐enrichment methods have emerged to boost sensitivity and enable easy detection of low‐frequency mutations. These methods are crucial in genomics research and clinical diagnostics, allowing for the detection of low‐frequency mutations within large genomic datasets. This review presents a summary of technological developments in rare mutation enrichment and emphasizes their mechanisms and applications in liquid biopsies.
Chiroptical Sensing of Amines With Isatins
Authors: Kariapper F. Safia , Miccolis Flavia , Pilicer Samantha L. , Wolf Christian
Published: October 2024

Isatins are extensively researched compounds with diverse applications, particularly as synthetic precursors in pharmaceutical developments. However, their use as optical probes for enantioselective sensing of chiral amines has not been explored to date. Herein, we present a novel chiroptical assay with an optimized isatin that generates strong, red‐shifted circular dichroism (CD) signals at approximately 380 nm upon ketimine formation with chiral amines. The intensity of the induced CD signal increases linearly with the enantiomeric excess of the analyte and thus allows quantitative chirality analysis. The general usefulness of this approach is demonstrated with a broad range of aliphatic and aromatic chiral amines, and by accurate determination of the enantiomeric composition of 10 samples.
Mechanism of TMB Discoloration Catalyzed by Layered CoNi@CN Nanozymes: Application Based on Smart Phone for Resorcinol Detection
Authors: Guo Qingyong , Xiao Rongsheng , Chen Haifeng , Bao Meishuo , Qi Jingwen , Jia Qian‐qian , Zhang Wuxiang
Published: October 2024

Comprehensive Summary

Real‐time on‐site monitoring of resorcinol (RS) concentrations is crucial for detecting hazardous levels, enabling prompt response measures to mitigate potential environmental and health risks. In this study, we developed an innovative method using CoNi@CN‐2 nanozymes to activate peroxymonosulfate (PMS) for oxidizing 3,3',5,5'‐tetramethylbenzidine (TMB). Our results show that the formation of Ni2+ through the oxidation of Ni0 on the CoNi@CN‐2 surface significantly enhances the electron‐donating capacity of Co0. The catalytic reaction of TMB is mediated by redox active species (SO4•−, •O2−, •OH and 1O2). RS drives colorimetry by transferring electrons to the benzene ring and specific nitrogen atoms in ox‐TMB, reducing ox‐TMB to TMB. Furthermore, the colorimetric assay shows a robust linear correlation between RS concentration and absorbance (Abs), described by Abs = –0.44[RS] + 0.886 (0—200 μmol/L, R2 = 0.983). Also, we introduce a novel smartphone‐integrated autonomous detection software that can analyze RS concentration and grayscale values (GSV), yielding GSV = 0.327[RS] + 63.601 (0—200 μmol/L, R2 = 0.990) with a detection limit of 5.29 μmol/L. Additionally, excess PMS leads to ROS attacking specific sites in ox‐TMB, forming secondary oxidation products. This study has enabled rapid and accurate detection of RS, making a significant contribution to environmental safety and protection.
Bushy‐Tailed Multicationic Quaternary Phosphonium Compounds: Potent Amphiphilic Disinfectants with Promising Therapeutic Indices
Authors: Rachii Diana , Bezold Elise L. , Wuest William M. , Minbiole Kevin P. C.
Published: October 2024

Quaternary ammonium compounds (QACs) have been essential for protecting human health for almost a century, functioning as surface disinfectants and sanitizers. With bacterial resistance increasing against commercially available QACs, the development of novel antimicrobials with divergent architectures is essential for effective infection prevention and control. Toward this end, our group has expanded beyond traditional ammonium scaffolds and explored the development of quaternary phosphonium compounds (QPCs). Herein, we report the synthesis and biological investigation of a series of 20 novel multicationic QPCs, bearing multiple short alkyl or aryl chains, also referred to as “bushy‐tailed” multiQPCs; these structures were hypothesized to have strong bioactivity while displaying low mammalian toxicity. Select bushy‐tailed QPC derivatives with trishexylphosphonium groups displayed single‐digit or sub‐micromolar activity against all seven bacteria tested, and MIC values of 2‐ to 8‐fold better than their bushy‐tailed QAC counterparts. Importantly, therapeutic indices of these bushy‐tailed QPCs were favorable in many cases, and were ≥4 against the entire bacterial panel for pX‐P6*,P6* and 1,8‐P6*,P6*, superior to more traditional architectures. This work highlights the promise of a novel set of multicationic phosphonium compounds as novel disinfectants with potent bioactivities and low toxicity.
Relative Bioavailability Studies With Mitapivat: Formulation and Food Effect Assessments in Healthy Subjects
Authors: Iyer Varsha , Sullivan Karen , Yan Yan , Hawkins Peter
Published: October 2024

Pyruvate kinase (PK) deficiency is a rare, hereditary, hemolytic anemia caused by mutations in the PKLR gene encoding the PK enzyme. Mitapivat (previously designated AG‐348) is a first‐in‐class, oral, allosteric activator of PK. We report results from 5 Phase 1 trials in healthy adults to characterize and compare mitapivat pharmacokinetics across different formulations and analyze food effects on mitapivat bioavailability (Studies 1‐5). Pharmacokinetic assessments were peak exposure, total exposure, time to maximum plasma concentration of mitapivat, and relative bioavailability (where appropriate). Plasma total exposure of mitapivat was similar in the fasted and fed (high‐fat meal or different soft foods) states after capsule, tablet, and pediatric granule formulations. Although mitapivat administration with food reduced the rate of mitapivat absorption (delay in time to maximum plasma concentration; reduction in maximum concentration) versus dosing under fasted conditions, this was not considered clinically relevant, given the lack of effect on total mitapivat exposure. Consequently, the administration instructions for mitapivat relating to food state that “patients may take mitapivat tablets with or without food.” These findings will continue to inform clinical studies and development of mitapivat in adult and pediatric patients with hemolytic anemias and may help inform healthcare professionals on mitapivat dosing/administration recommendations in clinical practice.
Synthesis of N3‐Methyluridine‐ and 2′‐O‐Alkyl/2′‐Fluoro‐N3‐Methyluridine‐Modified Phosphoramidites and Their Incorporation into DNA and RNA Oligonucleotides
Authors: Sahoo Avijit , Gore Kiran R.
Published: October 2024

In this article, we describe the synthesis of N3‐methyluridine (m3U) and 2′‐O‐alkyl/2′‐fluoro‐N3‐methyluridine (2′‐O‐alkyl/2′‐F‐m3U) phosphoramidites as well as their incorporation into a 14‐mer DNA and RNA oligonucleotide sequence. Synthesis of the 2′‐O‐alkyl‐m3U phosphoramidite starts with commercially available uridine to achieve a tritylated m3U intermediate, followed by 2′‐O‐alkylation and finally phosphitylation. Synthesis of the 2′‐F‐m3U phosphoramidite is obtained from a commercially available 2′‐F‐uridine nucleoside. These phosphoramidite monomers are compatible with DNA and RNA oligonucleotide synthesis using conventional phosphoramidite chemistry. This strategy offers efficient synthetic access to various modifications at the 2′‐position of m3U that can be employed in numerous nucleic acid–based therapeutic applications, including antisense technologies, small interfering RNAs, CRISPR‐Cas9, and aptamers. The data presented in this article are based on our previously published reports. © 2024 Wiley Periodicals LLC.

Basic Protocol 1: Synthesis of 2′‐O‐alkyl‐N3‐methyluridine analogs and their corresponding phosphoramidites

Alternate Protocol 1: Synthesis of 2′‐O‐TBDMS‐N3‐methyluridine and its phosphoramidite

Alternate Protocol 2: Synthesis of 2′‐fluoro‐N3‐methyluridine and its phosphoramidite

Basic Protocol 2: Solid‐phase synthesis of N3‐methyluridine‐modified DNA and RNA oligonucleotides
Contrasting effects of shooting disturbance on the movement and behavior of sympatric wildfowl species
Authors: Ozsanlav‐Harris Luke , McIntosh Aimée L. S. , Griffin Larry R. , Hilton Geoff M. , Cao Lei , Shaw Jessica M. , Bearhop Stuart
Published: October 2024

Human−wildlife conflict is a global conservation issue, necessitating effective mitigation strategies. Hunting is a common management approach to reduce conflict, but the indirect consequences are often overlooked. Chronic hunting‐related disturbance can reduce fitness and redistribute species. In recent decades, goose−agricultural conflict has intensified due to increasing abundance and shifts towards agricultural foraging. On Islay, Scotland, escalating conflict culminated in shooting Greenland barnacle geese Branta leucopsis to reduce damage to agricultural grassland. In this study, we contrast the impact of shooting disturbance on the movement, behavior, energy expenditure and habitat selection of the target species (Greenland barnacle goose) and a vulnerable nontarget species (Greenland white‐fronted goose, Anser albifrons flavirostris) using biologging devices (target species: n = 33; nontarget species: n = 94). Both species were displaced by shooting, and greater distances were subsequently traveled by the target species (1.71 km when directly targeted). When disturbed at any distance, total daily movement increased significantly by 1.18 km for the target species but not for the nontarget species. The target species exhibited no accompanying change in diurnal energy expenditure (measured via accelerometery) but foraged in improved grasslands further from roads after shooting disturbance, where disturbance from all sources was likely lower. The significant increases in movement and changes in foraging site selection of the target species could reduce fitness but given the infrequency of shooting disturbances (0.09 per day) there is likely capacity for compensatory feeding to recoup energetic losses. The nontarget species expectedly showed no significant change in energy expenditure, behavior or habitat selection following shooting disturbance, suggesting mitigation strategies have been effective at minimizing fitness impacts. Refuge areas with a 3.5 km diameter (three times the maximum distance from shooting that displacement was detectable) could provide undisturbed foraging for the target species, minimizing compensatory feeding and further agricultural damage. Wildlife managers should, where possible, consider the fitness implications of shooting disturbance, and whether compensatory feeding and redistribution could hamper conflict mitigation. Management strategies should also include species‐specific monitoring and mitigation as we have demonstrated differing responses potentially due to imposed mitigation but also differing species ecology and “landscapes of fear.”
Balancing Objective Markers and Subjective Experience in Eating Disorder Diagnoses: Commentary on Dang et al. (2024)
Authors: Hagan Kelsey E. , Christensen Pacella Kara A.
Published: October 2024

The results of Dang et al.'s recent systematic review and meta‐analysis suggested that individuals diagnosed with other specified feeding or eating disorder (OSFED) and those diagnosed with specified eating disorders (EDs, such as bulimia nervosa) endorse similar, elevated levels of ED‐related cognitions (but not behaviors). The DSM has traditionally conceptualized EDs primarily as disturbances in eating behavior, and the diagnostic boundaries for EDs are based on objective markers, such as behavioral frequencies and weight. Although focusing on objective markers for ED diagnoses and severity indices has advantages (e.g., clinical communication, measurement), pitfalls include diagnostic migration and low emphasis on ED cognitions. Dang et al.'s findings provide a basis for rethinking DSM's conceptualization of EDs as primarily behavioral. This commentary discusses the potential merits and challenges of emphasizing subjective cognitions when assigning ED diagnoses. We explore how objective markers (e.g., behavioral frequency, weight) and subjective experience (e.g., fear of weight gain) may be balanced to improve the clinical utility of ED diagnoses. In all, research that more deeply phenotypes the subjective experiences of people with EDs across contexts, identities, and cultures will enrich our understanding of eating pathology and may inform diagnostic revisions.
Taking a Deeper Dive Into OSFED Subtypes: A Meta‐Analysis and Systematic Review
Authors: Dang Thanh Ba , Hughes Elizabeth K. , Dang An Binh , Lai Heung Ying , Lee Jessica , Liu Shanshan , Portingale Jade , Fuller‐Tyszkiewicz Matthew , Krug Isabel
Published: October 2024

Objective

To compare all other specified feeding or eating disorders (OSFED) groups (atypical anorexia nervosa [AN], purging disorder [PD], night eating syndrome [NES], subthreshold bulimia nervosa [sub‐BN], and subthreshold binge‐eating disorder [sub‐BED]) to threshold eating disorders (EDs [AN, BN, and BED]) and control groups (CGs) on measures of eating and general psychopathology.

Method

We conducted a comprehensive search in PsycINFO, Medline, Embase, and CINAHL on all published studies from January 2013 to February 2024 using DSM‐5 diagnostic criteria via clinical interviews or well‐established diagnostic tools. We also undertook a quality appraisal using an adapted version of the Downs and Black criteria and registered the review with PROSPERO (ID: CRD42022314495).

Results

Overall, our meta‐analyses (n = 33 eligible studies) indicated that the combined OSFED and several specific OSFED subtypes displayed comparable levels of eating psychopathology to full‐threshold EDs. Our systematic review (n = 33 eligible studies) found individuals with OSFED to have comparable levels of eating and general psychopathology to full‐threshold EDs, but higher levels of eating and general psychopathology than CGs. These findings were specifically attributed to atypical AN and NES. There was a lack of evidence available for sub‐BN and sub‐BED. Studies mainly met the quality appraisal criteria. The main limitations identified in the included studies were insufficient reporting of their statistical power (78%) and no adjusting for potential confounding factors (67%).

Discussion

Findings support the conceptualization of atypical AN, and NES as clinically significant EDs with similar severity to full‐threshold EDs.