bluuebunny/crossref_metadata_2025 huggingface dataset:
Identification and Health Risks of an Emerging Means of Drug Use in Correctional Facilities
Authors: Kuai David , Rivera Blanco Liz Eneida , Krotulski Alex , Walton Sara , Denn Max , Kelly Byron , Kiernan Emily , Steck Alaina , Carpenter Joseph
Published: December 2024

Importance

Recreational use of drug-soaked paper strips (hereafter, strips) in correctional facilities poses a major public health risk owing to the diverse and potentially severe toxic effects of the substances they contain. Understanding the clinical manifestations and outcomes of exposure to these strips is important for developing effective management and prevention strategies.

Objective

To characterize the clinical manifestations, management, and outcomes of intoxication from strips in a correctional facility population, and to identify the specific substances present in these strips.

Design, Setting, and Participants

This is a case series with a retrospective medical record review and biospecimen analysis. Participants were incarcerated individuals from a county jail who presented to the emergency department of an urban hospital in Atlanta, Georgia, with suspected strip exposure between August 1, 2022, and November 1, 2023. Strip samples were tested using gas chromatography-mass spectrometry and liquid chromatography quadrupole time-of-flight mass spectrometry (LC-QTOF-MS), and serum samples were analyzed via LC-QTOF-MS.

Exposures

All patients had suspected exposure to strips, thought to contain opioids, synthetic cannabinoid receptor agonists (SCRAs), and other novel synthetic drugs.

Main Outcomes and Measures

The primary outcomes were clinical manifestations of strip exposure, including clinical signs and symptoms, vital sign derangements, laboratory and imaging findings, treatments administered, and patient outcomes.

Results

There were 18 patients (all male; median [IQR] age, 27.5 [18.0-45.0] years) in total. Bradycardia (11 patients [61%]) and central nervous system depression (17 patients [94%]) were the most common clinical findings. Other symptoms included agitation (6 patients [33%]) and seizures (4 patients [22%]). Treatment primarily involved supportive care, with 2 patients requiring intubation. One patient died as a result of hypoxic ischemic encephalopathy. Analysis of strip samples revealed the presence of synthetic cannabinoids and benzimidazole opioids, but no household cleaners or pesticides. Serum testing confirmed the presence of SCRAs and their metabolites.

Conclusions and Relevance

In this case series study of strip intoxication among incarcerated individuals, severe and variable clinical manifestations were observed, predominantly associated with their SCRA content. Bradycardia in the context of major central nervous system depression was an indicator of severe SCRA toxic effects. Further research is needed to better understand strip use and to develop effective prevention and treatment strategies.
The FEBS 60th anniversary writing contest—blueprints for the scientific society of tomorrow
Authors: Wright Duncan E.
Published: December 2024

The Federation of European Biochemical Societies (FEBS) celebrated its 60th anniversary in 2024, and FEBS Letters marked the occasion with a writing contest on the future of scientific societies. This editorial introduces the winning article by Yussuf Ali and presents an overview of the predominant themes that emerged during the contest, which included AI, interdisciplinarity, diversity and sustainability.
Synthesis and Reactivity of Fluorinated Organometallic Species
Authors: Rueda‐Espinosa Juan , Love Jennifer A.
Published: December 2024

This chapter aims to serve as an introduction to recent advances (2015–2022) in the synthesis of fluorinated organometallic species and the study of their reactivity. Each section focuses on metal complexes bearing metal–fluoride bonds (MF), metal–polyfluoroalkyl bonds (MRF), and fluorinated arenes. These sections are structured in terms of conceptually different synthetic approaches and reactivity patterns. Thermodynamic and mechanistic considerations of the synthesis and reactivity of these species are discussed where possible.
Treatment Response Biomarkers for Systemic Sclerosis–Associated Interstitial Lung Disease
Authors: Volkmann Elizabeth R. , Wilhalme Holly , Tashkin Donald P. , Kim Grace Hyun J. , Goldin Jonathan , Haussmann Alana , Kuwana Masataka , Roth Michael D. , Assassi Shervin
Published: December 2024

Objective

This study investigated whether changes in circulating biomarkers predict progressive pulmonary fibrosis (PPF) in patients with systemic sclerosis–associated interstitial lung disease (SSc‐ILD) receiving treatment.

Methods

Participants of the Scleroderma Lung Study II, which compared receiving mycophenolate mofetil (MMF) versus cyclophosphamide (CYC) for treating SSc‐ILD, who had blood samples at baseline and 12 months were included. Levels for C‐reactive protein (CRP), interleukin‐6, C‐X‐C motif chemokine ligand (CXCL) 4, CCL18, and Krebs von den Lungen (KL)‐6 were measured, and a logistic regression model evaluated relationships between changes in these biomarkers and the development of PPF by 24 months.

Results

A total of 92 of the 142 randomized participants had longitudinal biomarker measurements and the required clinical outcome data, with 19 participants (21%) meeting criteria for PPF. In the whole cohort, changes in KL‐6 levels were significantly correlated with PPF. KL‐6 increased in patients who developed PPF and decreased in patients who did not (mean change ± SD 365.68 ± 434.41 vs −207.45 ± 670.26; P < 0.001). In the arm of participants who received MMF alone, changes in CRP and CXCL4 levels were also significantly correlated with PPF. When added to an existing prediction model based on baseline factors associated with PPF in this cohort (sex, baseline reflux severity, and CXCL4 levels), the change in KL‐6 remained significantly associated with PPF (odds ratio 1.4; P = 0.0002).

Conclusion

Changes in the circulating levels of KL‐6 after treatment with MMF or CYC predicted PPF, even after adjusting for baseline factors associated with PPF. Measuring longitudinal KL‐6 in patients with SSc‐ILD may improve how we personalize therapy in patients with SSc‐ILD.
Gout Flares After Stopping Anti‐Inflammatory Prophylaxis: A Rapid Literature Review and Meta‐Analysis
Authors: Stamp Lisa K. , Frampton Christopher , Newcomb Jeff A. , O'Dell James R. , Mikuls Ted R. , Dalbeth Nicola
Published: December 2024

Objective

The aim of this research was to determine how common gout flares are after ceasing anti‐inflammatory prophylaxis.

Methods

A rapid literature review and meta‐analysis were undertaken. PubMed was searched from inception to February 2024. Eligibility criteria included any clinical trial of people with gout with at least one arm starting or intensifying urate‐lowering therapy (ULT) with coprescription of anti‐inflammatory prophylaxis and that had the percentage of participants experiencing one or more gout flares reported during and after the period of prophylaxis. Random effects meta‐analyses were used to generate pooled estimates of the percentage of participants experiencing one or more flares in each period.

Results

Six trials were included, together with aggregated, unpublished data from the VA STOP Gout trial (2,972 participants). Pooled random effects estimates of the percentage of participants having one or more gout flares were 14.7% (95% confidence interval [CI] 11.3–18.5%) during prophylaxis, 29.7% (95% CI 22.9–37.0%) in the three‐month period after ceasing prophylaxis, and 12.2% (95% CI 6.8–19.0%) during the last study period. The mean difference in the percentage of participants having one or more gout flare while taking prophylaxis and immediately after ceasing prophylaxis was −14.8.0% (95% CI −21.2% to −8.5%; P < 0.0001). The mean difference from the period immediately following prophylaxis discontinuation compared to the last study period was 16.0% (P < 0.001). Sensitivity analyses indicated no material effects of prophylaxis duration, trial duration, ULT class, or placebo arms.

Conclusion

Gout flares are common after stopping anti‐inflammatory prophylaxis but return to levels seen during prophylaxis. Patients should be cautioned about the risk of gout flares and have a plan for effective gout flare management in the three months after stopping anti‐inflammatory prophylaxis.
Movement Pattern Biofeedback Training After Total Knee Arthroplasty: A Randomized Controlled Trial
Authors: Bade Michael J. , Christiansen Cory L. , Zeni Joseph A. , Dayton Michael R. , Forster Jeri E. , Cheuy Victor A. , Christensen Jesse C. , Hogan Craig , Koonce Ryan , Dennis Doug , Peters Amy , Stevens‐Lapsley Jennifer E.
Published: December 2024

Objective

Habitual movement compensations, such as decreased surgical peak knee extension moments (pKEM), persist years after total knee arthroplasty (TKA), are linked to poorer recovery, and may influence contralateral osteoarthritis progression. The purpose of this randomized clinical trial was to determine if a movement training program (MOVE) improves movement quality and recovery after TKA compared to a standardized rehabilitation program without movement training (CONTROL).

Methods

One hundred thirty‐eight individuals were randomized to either MOVE or CONTROL groups after TKA. Participants were assessed preoperatively, 10 weeks after (end of intervention), and six months after (primary endpoint) TKA. Outcomes assessed were pKEM during walking, six‐minute walk test, stair climb test, 30‐second sit to stand test (30STS), timed up and go test (TUG), physical activity level, strength, range of motion, and self‐reported outcomes.

Results

At six months, there were no between‐group differences in surgical pKEM during walking (primary outcome). The MOVE group exhibited less contralateral pKEM compared to CONTROL during self‐selected gait speed (d = 0.44, P = 0.01). CONTROL performed better on TUG and 30STS at 10 weeks (P < 0.05), but differences attenuated at six months.

Conclusion

The MOVE intervention did not lead to improved surgical pKEM during walking after TKA compared to CONTROL. However, the MOVE group did demonstrate less contralateral pKEM during walking. The CONTROL group demonstrated faster recovery on the TUG and 30STS, but it is unknown if this is due to improved recovery in the surgical knee or increased movement compensation relying on contralateral knee function.
A Universal Strategy for Microcapsule Diversity via Interfacial Surfactant Complexation in Fluorocarbon Oil‐Based Triple Emulsions
Authors: Lee Je Hyun , Choi Chang‐Hyung , Lee Hyomin
Published: December 2024

Microfluidic emulsion‐templating offers the preparation of functional microcapsules with tunable compositions and structures that are otherwise inaccessible using conventional methods. However, the inherent nature of emulsions relying on the immiscibility of phases comprising the emulsion limits the use of a single platform for the realization of microcapsules with diversity in shell materials. Herein, fluorocarbon oil‐based triple emulsions are utilized as templates to achieve microcapsule diversity through a single platform. By introducing fluorocarbon oil with omniphobicity as the interstitial phase between the core and the shell phase, additional degrees of freedom are provided in the library of shell materials applicable in the design of functional microcapsules. Moreover, it is demonstrated that surfactant complexation at the emulsion interface effectively enhances the stability of the emulsion. This grants the use of various solidification methods including polymerization, freezing, and even solvent removal without delicate control of spreading coefficients or complex surfactant synthesis processes. The showcased microcapsule diversity signifies pivotal breakthroughs in microencapsulation technologies, illustrating how the synergistic use of fluorocarbon oil and interfacial complexation of surfactants in emulsions provides true freedom in universal microcapsule shell design for various applications including cosmetics, food, drug delivery, and cell therapy to name a few.
A Facile Humidity‐Induced Porous Framework Filled with In Situ Initiated Gel Electrolyte for Stabilizing Li1.3Al0.3Ti1.7(PO4)3/Li Interface
Authors: Yang Dezhi , Yang Yanan , Sun Yiyang , Zhang Tao
Published: December 2024

NASICON‐type Li1.3Al0.3Ti1.7(PO4)3 (LATP) is a highly competitive solid‐state electrolyte due to its high ionic conductivity, nice air stability, and low cost. However, the interface failure resultingfrom the continuous side reaction between LATP and lithium anode limits its further development. Here, a humidity‐induced porous polyvinylidene fluoride (PVDF) framework filled with in situ initiated poly(1,3‐dioxolane) (PDOL)‐based gel electrolyte is developed to stabilize LATP/Li interface. The porous PVDF framework isolates the direct contact between LATP and Li. The internally filled PDOL‐based gel electrolyte contributes to the smooth and uniform Li+ plating/stripping, which mitigates the interfacial side reaction induced by lithium dendrite penetration. In addition, the used ring‐opening polymerization initiator, Zn(OTf)2, is reduced on the lithium anode to form Li‐Zn alloy which further optimizes Li+ transport. Lithium symmetrical cells assembled with the modified LATP above can stably operate for over 1800 h at 0.1 mA cm−2. Also, LFP‐based solid‐state lithium batteries assembled with the modified LATP represent a favourable capacity retention of 94.8% for 700 cycles at 0.2C and 92% for 400 cycles at 0.5C. This work provides a facile organic interface strategy to realize stable LATP/Li interface and shows the promising potential to be universally applicable for stabilizing various rigid and unstable electrolyte/Li interface.
Copolymerization of Poly (Triazine Imide) Single Crystal Nanoplates with Enhanced Charge Transfer for Efficient Photocatalytic Overall Water Splitting
Authors: Zou Guirong , Wang Qian , Ye Gui , Pan Zhiming , Wang Sibo , Anpo Masakazu , Zhang Guigang
Published: December 2024

Solar‐driven photocatalytic overall water splitting represents a sustainable strategy to produce green hydrogen using metal‐free polymeric carbon nitride. However, conventional thermal polymerization with a single precursor for the synthesis of poly (triazine imide) faces challenges such as slow deamination rates and mass transfer, resulting in the formation of undesired structural defects, which usually serve as charge recombination sites and decrease the photocatalytic performance. Herein, highly crystalline poly (triazine imide) by thermal copolymerization of binary precursors of melamine and cyanuric acid in the presence of molten salts is reported. The results reveal that melamine and cyanuric acid easily generate melam (intermediates of carbon nitride) and subsequently facilitate the polycondensation process. Solid characterizations revealed that crystalline poly (triazine imide) nanoplates with extended π‐conjugation degrees and reduced intensity of structural defects would be obtained, which largely promotes separation and migration of photogenerated carriers, and inhibits the undesirable charge recombination at the defect sites. Accordingly, after in situ photo‐deposition of CoOx and Pt/Cr2O3 as O2 and H2 evolution co‐catalysts, respectively, the optimized crystalline poly (triazine imide) nanoplates achieve an excellent solar‐to‐hydrogen conversion of 0.30% under simulated sunlight irradiation.
Synergistic Effects of Ruthenium and Zinc Active Sites Fine Tune the Electronic Structures of Augmented Electrocatalysis
Authors: Lu Tingyu , Li Jing , Ying Jingwen , Peng Ningkang , Zhang Linda , Zhang Yizhou , Zhang Di , Ye Songbo , Xu Lin , Sun Dongmei , Li Hao , Gu Yanhui , Tang Yawen
Published: December 2024

As the demand for cleaner energy becomes a paramount objective of sustainable development, the advancement of cutting‐edge engineered materials for a wide range of applications becomes increasingly vital. Tailoring catalyst properties through precise design and electronic state tuning is essential for adapting these materials to large‐scale energy applications. Given this, an effective electronic fine‐tuning (EFT) strategy is presented to optimize the electronic structures of single‐atom Zn site and Ru species, synergistically enhancing the both electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Benefiting from the interaction between Ru species anchored on hierarchically layered nanosheets and isolated Zn atoms (Ru@Zn‐SAs/N‐C), the catalyst exhibits superior ORR and HER activities compared to the benchmark Pt/C catalyst. X‐ray absorption spectroscopy and density functional theory (DFT) calculations confirm a novel EFT effect between a single Zn site and Ru species, that enables the Ru@Zn‐SAs/N‐C approaches the optimal scaling relation between *OOH and *OH, breaking the universal ORR scaling limitation. Additionally, the optimal GH* value positions Ru@Zn‐SAs/N‐C near the apex of the theoretical HER volcano model. This work provides an innovative avenue for regulating the electronic localization of catalytic active centers by virtue of carbon substrate and offers valuable insights for designing high‐efficiency electrocatalysts.
Controlled Release of Human Dental Pulp Stem Cell‐Derived Exosomes from Hydrogels Attenuates Temporomandibular Joint Osteoarthritis
Authors: Diez‐Guardia Victor , Tian Yajing , Guo Yunzhe , Li Jiaying , Cui Shengjie , Dreiss Cécile A. , Gentleman Eileen , Wang Xuedong
Published: December 2024

Temporomandibular joint osteoarthritis (TMJOA) is a painful inflammatory condition that limits mouth opening. Cell‐derived exosomes, which have anti‐inflammatory effects, are emerging as a treatment for TMJOA. Injection of dental pulp stem cells (DPSCs), which secrete exosomes, can moderate tissue damage in a rat model of TMJOA. However, injected exosomes are quickly cleared, necessitating repeated injections for therapeutic efficacy. Here, vinyl sulfone‐modified hyaluronic acid (HA‐VS) hydrogels, suitable for encapsulating exosomes are formulated. HA‐VS hydrogels degrade in the presence of hyaluronidase and allow for the release of beads of similar size to exosomes over 3 to 6 days. In a rat model of TMJOA, injection of exosomes or exosomes within HA‐VS hydrogels significantly attenuated damage‐mediated subchondral bone loss as determined by micro‐computed tomography, and reduced inflammatory and tissue damage scores as assessed by histology. Overall, DPSCs‐derived exosomes attenuated joint damage, but treatment with exosomes within HA‐VS hydrogels shows additional protective effects on subchondral bone maintenance and integrity. These findings confirm the protective effects of DPSCs‐derived exosomes in moderating tissue damage in TMJOA and suggest that combining exosomes with HA hydrogels can further promote their therapeutic effects.
Amorphous High‐entropy Phosphide Nanosheets With Multi‐atom Catalytic Sites for Efficient Oxygen Evolution
Authors: Li Xiumin , Xie Zhengkun , Roy Soumyabrata , Gao Longqing , Liu Jie , Zhao Bing , Wei Ran , Tang Bijun , Wang Hongyan , Ajayan Pulickel , Tang Keyong
Published: December 2024

The alkaline oxygen evolution reaction (OER) mainly encompasses four elementary reactions, involving intermediates such as HO*, O*, and HOO*. Balancing the Gibbs free energies of these intermediates at a single active site is a challenging task. In this work, a high‐entropy metal‐organic framework incorporating Fe, Ni, Co, Cu, and Y metal elements is synthesized using an electrodeposition method, which then serves as a template for preparing a high‐entropy phosphide/carbon (FeCoNiCuYP/C) composite. Notably, the obtained composite exhibits an amorphous structure with multiple catalytically active sites. Combined theoretical calculations and experimental measurements reveal the critical roles of Co/Ni and Fe atoms in tuning the electronic structure of FeCoNiCuYP and optimizing the binding strength of intermediates. Furthermore, Fe and Ni/Co sites prefer to stabilize the HO* and HOO* intermediates respectively, conducive to breaking their scaling relation of Gibbs free energy during OER. Owing to its fine‐tuned composition and the synergistic effect of multiple active sites, the FeCoNiCuYP/C electrocatalyst demonstrates superior OER performance in alkaline solutions, requiring a mere 316 mV overpotential to yield 100 mA cm−2 current density with excellent stability. This work provides an innovative route to design efficient high‐entropy electrocatalysts, holding significant promise for cutting‐edge electrocatalytic applications.
Self‐Assembled Metal Complexes in Biomedical Research
Authors: Wang Wenting , Xu Yang , Tang Yuqi , Li Quan
Published: December 2024

Cisplatin is widely used in clinical cancer treatment; however, its application is often hindered by severe side effects, particularly inherent or acquired resistance of target cells. To address these challenges, an effective strategy is to modify the metal core of the complex and introduce alternative coordination modes or valence states, leading to the development of a series of metal complexes, such as platinum (IV) prodrugs and cyclometalated complexes. Recent advances in nanotechnology have facilitated the development of multifunctional nanomaterials that can selectively deliver drugs to tumor cells, thereby overcoming the pharmacological limitations of metal‐based drugs. This review first explores the self‐assembly of metal complexes into spherical, linear, and irregular nanoparticles in the context of biomedical applications. The mechanisms underlying the self‐assembly of metal complexes into nanoparticles are subsequently analyzed, followed by a discussion of their applications in biomedical fields, including detection, imaging, and antitumor research.
High‐Yield, Cost‐Effective Fabrication of High‐Aspect‐Ratio Polyimide Microstructures for Robust Superhydrophobic Surfaces
Authors: Jeung Jinpyeo , Yun Inyeol , Park Hyuk , Chung Yoonyoung
Published: December 2024

Superhydrophobic surfaces (SHS), with their exceptional water‐repellent properties, have attracted great interest due to their versatile applications. The robustness of SHS has emerged as an essential issue for practical applications, as SHS are directly exposed to various harsh environments, such as continuous raindrop impact, corrosive media, and extreme temperatures. Polyimide (PI) is an ideal candidate for robust SHS due to its superior mechanical, thermal, and chemical properties. However, the low processability of PI in surface microstructuring has limited its application in SHS. In this study, a high‐yield and cost‐effective fabrication method for constructing high‐aspect‐ratio PI microstructures has been developed by controlling the template surface treatment, precursor molecular weight, and vacuum process. This approach achieves an exceptional yield rate of 99.8% and an aspect ratio of 10.7, enabling the construction of various microstructures. The SHS is demonstrated by fabricating microstructures on PI surfaces using the proposed method. The PI SHS exhibits a water contact angle of up to 162° and a roll‐off angle of less than 9°. The water repellency withstands 100 tape peeling tests and remains stable after continuous exposure to temperatures up to 250 °C and various chemical reagents for 60 days, which presents excellent robustness against environmental factors.
High‐Resolution Patterning and Efficient Fabricating of Liquid Metal Microelectrodes Using PNIPAM Sacrificial Layer
Authors: Liu Xing , Zheng Jiahui , Xu Xiaoyun , Hao Shilei , Hu Ning , Zheng Xiaolin
Published: December 2024

Microelectrodes play a crucial role in microfluidic chips. However, electrodes with micron‐sized geometries lead to undesired impedance increases and processing difficulties. This study introduces a method for preparing low‐resistance and low‐cost liquid metal microelectrodes (), which leverages the distinct phase transition properties of liquid metal (LM) gallium (Ga) and Poly‐N‐Isopropylacrylamide (PNIPAM), along with the reversible bonding between PNIPAM and polydimethylsiloxane (PDMS). PNIPAM is spin‐coated as a sacrificial layer on silanized glass and heated to dehydration. As it hydrates and swells in the water bath, Ga/PDMS can be easily peeled off, forming a precision surface‐embedded . The resistance of the with a thickness of 25 was only 9.3% and 0.077% of the 100nm thin film Au and indium tin oxide (ITO) film microelectrode with the same plane size. Hydration and swelling of the sacrificial layer ensured the fabrication with high resolutions down to 5 and an acute angle of 15°. The electroosmotic flow tests show that the effectively reduces the operating voltage compared to conventional planar Au or ITO microelectrodes. These features make it a promising candidate for electrification requirements in microfluidic devices.
Highly Sensitive InSe Nanosheet Ultraviolet Photodetector Realized Via an Asymmetric Fabry–Pérot Structure
Authors: Chen Shi‐Rong , Shan Long‐Qiang , Shu Wei , Liang Li‐Yan , Wang Jiang , Hu Ji‐Gang , Zhu Wen‐Huan , Luo Lin‐Bao , Wu Chun‐Yan
Published: December 2024

Due to the wavelength‐dependent absorption, narrow bandgap semiconductors show potential application in ultraviolet (UV) photodetection by thinning. However, the limited absorption in the thinner layer retards their application in high‐performance photodetection. In this paper, the fabrication of an asymmetric Fabry–Pérot (F–P) structure is reported by planar stacking of InSe layer, Al2O3 spacer, and Al back reflector. For the selective absorption enhancement in UV region, the Al2O3 thickness is optimized to be 39 nm by finite element method (FEM). The device presents a peak response at 265 nm illumination, showing the photo‐to‐dark current ratio (Ilight/Idark) of 719. Responsivity (R) and photoconductive gain (G) reach 11.7 A W−1 and 54.7 at the weak light intensity of 0.03 mW cm−2, respectively, which are two orders of magnitude higher than those of the device without the asymmetric F–P structure, revealing the remarkably enhanced absorption. This work shows well compatibility with the manufacturing processes for 2D semiconductor‐based photodetectors and provides a simple and versatile strategy for the application of 2D narrow bandgap semiconductors in high‐performance UV photodetectors.
Synthesis of Bishomocubanone Derivatives via Visible‐Light‐Induced Intramolecular [2+2] Cycloaddition Reaction
Authors: Yan Bingning , Zhang Qingzhong , Ling Yifei , Liu Jiaxin , Yang Jun
Published: December 2024

In this paper, a visible‐light‐induced intramolecular [2+2] cycloaddition has been revealed to synthesize the bishomocubanone derivatives in moderate to excellent yield under mild conditions. This method demonstrated a broad substrate scope and excellent functional‐group tolerance, affording cubane precursors and a series of bishomocubanones. Meanwhile, a hundred‐gram scale experiment of this method has been employed to synthesize cubane precursors with 98% yield.
Iron Catalyzed Radical Alkylation of Cyclic Ketimines with Olefins via Metal Hydride Atom Transfer
Authors: Hu Xixi , Sun Ruizhi , Tian Yu , Xu Xinyue , Zhu Yijia , Liu Hui , Liu Dong , Zhang Lizhi
Published: December 2024

Here, we present an innovative approach to achieve Minisci‐type alkylation of cyclic N‐ketimines, enabling access to a diverse range of valuable alkylated sulfonyl ketimines via iron hydride hydrogen atom transfer. More than 35 examples are shown with a wide range of substrates. Additionally, this system is easy to operate and can be efficiently scaled up. Mechanistic investigations revealed that the alkyl radical process involved and the air acts as the sole oxidant in this system.
Thermal Noise‐Induced Phase Transition in Multi‐Domain Hf‐Based Antiferroelectric Material: Fatigue and Endurance Performance
Authors: Luo Sheng , Zheng Zijie , Zhou Zuopu , Gong Xiao , Liang Gengchiau
Published: December 2024

The deterioration of the endurance performance in the Hf‐based antiferroelectric (AFE) material is a crucial challenge in the reliability of its device applications, and it is important to identify the mechanism for further optimizations. In this work, a stochastic AFE dynamic model is proposed to characterize the fatigue behaviors induced by thermal noise‐induced lattice vibration. Through the analysis of the noise‐assisted phase transition between the antiferroelectric and ferroelectric (FE) phases, the impact of the thermal effect on endurance is evaluated and the results are in good agreement with the experiments. Both temperature and dipole coupling strength are found to be the key factors in noise‐induced fatigue. Furthermore, the thermal noise‐induced stochastic dynamics is found to have a profound impact in the AFE‐based memory's reliability, and the memory window demonstrates direct dependency on temperature and domain dynamics.
Enhance Charge Transfer and Reduce Internal Resistance for Triboelectric Nanogenerator via Switching Charge Shuttling
Authors: Guo Xin , Wang Yuqi , Feng Yuming , Yu Yang , Wang Jianlong , He Siyang , Zhu Jinzhi , Li Hengyu , Cheng Tinghai , Wang Zhong Lin , Cheng Xiaojun
Published: December 2024

Traditional triboelectric nanogenerators (TENGs) face significant challenges related to low charge density and high internal impedance. Many methods have been proposed to enhance the surface charge density of TENGs, yet they do not simultaneously achieve low internal resistance. Here, a switch‐shuttling triboelectric nanogenerator (SS‐TENG) is proposed. By periodically interrupting the circuit during the intrinsic capacitance variation of the TENG during the charge shuttle process, the SS‐TENG alters the potential difference while maintaining a constant charge in the capacitor, thereby enhancing energy storage and improving overall output performance. The rapid activation of the switch significantly reduces internal resistance. Compared to traditional charge shuttle TENGs, the charge transfer amount increases by 1.9 times, while the short‐circuit current rises by 9.6 times, with internal resistance reduced by a factor of 20. Furthermore, a prototype of the novel cylindrical‐hexagram bluff body (CHB) vortex‐induced vibration energy harvester based on the SS‐TENG is designed and tested, demonstrating its ability to reliably harvest energy from underwater tidal flows and surface wave energy. Additionally, a self‐powered marine pollution detection strategy has been developed using the SS‐TENG. This work provides valuable insights for enhancing the performance of TENGs and actively promotes their commercialization.
Long‐Distance Autonomous Navigation of Optical Microrobotic Swarms in Complex Environments
Authors: Chen Zhihan , Huang Siyuan , Zheng Yuebing
Published: December 2024

The local force field generated by light endows optical microrobots with remarkable flexibility and adaptivity, promising significant advancements in precise medicine and cell transport. Nevertheless, the automated navigation of multiple optical microrobots in intricate, dynamic environments over extended distances remains a challenge. Herein, a versatile control strategy aimed at navigating optical microrobotic swarms to distant targets under obstacles of varying sizes, shapes, and velocities is introduced. By confining all microrobots within a manipulation domain, swarm integrity is ensured while mitigating the effects of Brownian motion. Obstacle's elliptical approximation is developed to facilitate efficient obstacle avoidance for microrobotic swarms. Additionally, several supplementary functions are integrated to enhance swarm robustness and intelligence, addressing uncertainties such as swarm collapse, particle immobilization, and anomalous laser–obstacle interactions in real microscopic environments. We further demonstrate the efficacy and versatility of our proposed strategy by achieving autonomous long‐distance navigation to a series of targets. This strategy is compatible with both optical trapping‐ and nudging‐based microrobotic swarms, representing a significant advancement in enabling optical microrobots to undertake complex tasks such as drug delivery and nanosurgery and understanding collective motions.
Familial RPL26 Variant Causing Congenital Anomalies Without Hematological Features of Diamond Blackfan Anemia
Authors: Karger Lisa M. , Webb Bryn D. , Edelmann Lisa , Liao Jun , Mehta Lakshmi
Published: December 2024

Diamond Blackfan anemia (DBA) is an autosomal dominant disorder with a heterogeneous clinical presentation which may include macrocytic anemia typically presenting in the first year of life, growth retardation, and congenital malformations in 30%–50% of patients. This phenotypic variability is partially explained by genotype–phenotype correlations, with several ribosomal protein genes implicated in this disorder. Most cases are due to de novo variants, but familial occurrences highlight variable expressivity and reduced penetrance. To date, one case has been previously reported with a pathogenic variant in the RPL26 gene: a 3.5‐year‐old female with multiple congenital anomalies and typical hematological features of DBA. Here, we report a novel frameshift variant in RPL26 identified in a proband and his brother with limb malformations without anemia. Decreased RPL26 protein levels were detected in the proband's lymphoblasts. Subsequent clinical workup revealed high erythrocyte adenosine deaminase activity (eADA) in the proband, without anemia. This family represents the second report of RPL26‐associated congenital anomalies in the DBA spectrum and further illustrates the non‐hematological presentation of Diamond Blackfan “anemia”.
On the Photoisomerization of Pyridine in Vapor Phase
Authors: D'Auria Maurizio
Published: December 2024

DFT calculations on the photoisomerization of pyridine, 2,3‐, 2,6, and 3,4‐dimethylpyridine showed that the photoisomerization occurs through the formation of the corresponding Dewar isomers. These compounds can be transformed into the corresponding benzvalene isomers, whose decomposition gives the reaction products. Another way to obtain some observed reaction products is a photoisomerization of the Dewar isomers through an intramolecular thermal or photochemical [2+2]‐cycloaddition reaction.
Alzheimer's Association clinical practice guideline for the Diagnostic Evaluation, Testing, Counseling, and Disclosure of Suspected Alzheimer's Disease and Related Disorders (DETeCD‐ADRD): Executive summary of recommendations for primary care
Authors: Atri Alireza , Dickerson Bradford C. , Clevenger Carolyn , Karlawish Jason , Knopman David , Lin Pei‐Jung , Norman Mary , Onyike Chiadi , Sano Mary , Scanland Susan , Carrillo Maria
Published: December 2024

US clinical practice guidelines for the diagnostic evaluation of cognitive impairment due to Alzheimer's disease (AD) or AD and related dementias (ADRD) are decades old and aimed at specialists. This evidence‐based guideline was developed to empower all—including primary care—clinicians to implement a structured approach for evaluating a patient with symptoms that may represent clinical AD/ADRD. Through a modified‐Delphi approach and guideline‐development process (7374 publications were reviewed; 133 met inclusion criteria) an expert workgroup developed recommendations as steps in a patient‐centered evaluation process. This summary focuses on recommendations, appropriate for any practice setting, forming core elements of a high‐quality, evidence‐supported evaluation process aimed at characterizing, diagnosing, and disclosing the patient's cognitive functional status, cognitive–behavioral syndrome, and likely underlying brain disease so that optimal care plans to maximize patient/care partner dyad quality of life can be developed; a companion article summarizes specialist recommendations. If clinicians use this guideline and health‐care systems provide adequate resources, outcomes should improve in most patients in most practice settings.

Highlights

US clinical practice guidelines for the diagnostic evaluation of cognitive impairment due to Alzheimer's disease (AD) or AD and related dementias (ADRD) are decades old and aimed at specialists.

This evidence‐based guideline was developed to empower all—including primary care—clinicians to implement a structured approach for evaluating a patient with symptoms that may represent clinical AD/ADRD.

This summary focuses on recommendations, appropriate for any practice setting, forming core elements of a high‐quality, evidence‐supported evaluation process aimed at characterizing, diagnosing, and disclosing the patient's cognitive functional status, cognitive–behavioral syndrome, and likely underlying brain disease so that optimal care plans to maximize patient/care partner dyad quality of life can be developed; a companion article summarizes specialist recommendations.

If clinicians use this guideline and health‐care systems provide adequate resources, outcomes should improve in most patients in most practice settings.
Life's Essential 8 and midlife trajectories in cognition and brain health: The CARDIA study
Authors: Dintica Christina Silvia , Jiang Xiaqing , Launer Lenore J. , Bryan R. Nick , Yaffe Kristine
Published: December 2024

INTRODUCTION

Poor cardiovascular health (CVH) is linked to Alzheimer's disease and dementia; however, its association with neurocognitive trajectories earlier in life remains underexplored.

METHODS

We included 3224 participants with information on CVH at early midlife (mean age 45.0 ± standard deviation 3.4) an cognitive assessments, and neuroimaging 5, 10, and 15 years later including white matter hyperintensities (WMHs), total gray matter (GM), and hippocampal volume. CVH was operationalized according to the American Heart Association's (AHA) “Life's Essential 8” (LE8) guidelines. The association between LE8 and cognitive and neuroimaging measures was examined using mixed linear regression adjusting for age, sex, race, and education.

RESULTS

Worse LE8 score was associated with steeper decline in cognition, higher accumulation of WMHs, and steeper decline in total GM and hippocampal volume.

DISCUSSION

Poor CVH is related to accelerated brain aging across midlife, highlighting the need to screen for and improve CVH earlier to prevent adverse cognitive outcomes.

Highlights

Poor cardiovascular health in early midlife is associated with faster decline in cognition across 10 years overall and in specific domains.

Poor and intermediate cardiovascular health was associated with higher accumulation of white matter hyperintensities across midlife.

Poor cardiovascular health was associated with faster atrophy in total gray matter volume and hippocampal volume.
The Interplay Between Component Denticity and Flexibility Promotes the Formation of [AgI⋅⋅⋅AgI]‐stabilised Links and Knots
Authors: Sarwa Aleksandra , Khmara Andrei , Konieczny Krzysztof A. , Kulesza Dagmara , Zych Eugeniusz , Trzaskowski Bartosz , Szyszko Bartosz
Published: December 2024

A subtle interplay between the flexibility of the 2,2’‐bipyridyl‐based diamine and the denticity of the coordination domain formed upon self‐assembly enabled the formation of four distinct topologies stabilised by [Ag⋅⋅⋅Ag]2+ pairs. The reactions utilising 2,6‐diformylpyridine resulted in the formation of silver(I)‐stabilised molecular tweezer, trefoil knot, and Solomon link. The 1,8‐naphthyridine‐based dialdehyde promoted the formation of [2]catenanes and trefoil knot, demonstrating very close AgI⋅⋅⋅AgI distances. Two of the studied assemblies demonstrated interesting luminescent properties in the solid state.
Synergistic Enhancement of Plasma‐Driven Ammonia Synthesis Using a AuCu3/Cu Composite Catalyst
Authors: Li Zhenlu , Liu Shize , Zhan Qingyun , Li Jiayang , Zhang Zihao , Qian Yumeng , Cai Yiyu , Mu Xiaoyue , Li Lu
Published: December 2024

Green ammonia synthesis using fluctuating renewable energy supply in decentralized process is a goal that has been long sought after. Ammonia synthesis with non‐thermal plasma under mild conditions is a promising technology, but it faces the critical challenge of low energy efficiency. Herein, we develop an easily‐scalable AuCu3/Cu catalyst, which consists of a decimeter‐scale metallic Cu antenna and nano‐scale AuCu3 catalytic sites on metallic Cu surface, significantly enhancing the energy efficiency and ammonia yield in a radio‐frequency (RF) plasma system. Compared to plasma alone, the single‐pass ammonia yield over AuCu3/Cu increases by a factor of 20, approaching 10 %. Mechanistic studies indicate that Cu antenna can amplify the millimeter‐scale local electric field, thereby facilitating the generation of active nitrogen species, including nitrogen radicals and vibration‐excited nitrogen molecules. Due to the downshifted d‐band center and unique Cu−Au interface structure, the AuCu3 nanoalloy modified on Cu antenna surface significantly reduces hydrogenation barriers of active NHX (x=0,1,2) species (the rate‐determining step) and facilitates ammonia desorption at lower temperature. The synergistic effect of Cu antenna and surface AuCu3 nanoalloy comprehensively enhances ammonia synthesis through both the nitrogen radical‐mediated Eley‐Rideal pathway and the vibration‐excited nitrogen molecule‐mediated Langmuir–Hinshelwood pathway.
Molecular Customization of Anode‐Electrolyte Interfaces for Enhanced Stability and Reversibility in Aqueous Zinc‐Carbon Capacitors
Authors: Xu Yang , Chen Jingzhu , Li Tao , Ma Hexian , Lv Zhuoran , Zhang Shicong , Bi Hui , Huang Fuqiang , Lin Tianquan
Published: December 2024

Aqueous zinc‐carbon capacitors display application potential in green power and high‐end equipment owing to their high security, large power and sustainability. The water‐rich zinc anode‐electrolyte interface (AEI) and disordered zinc‐ion diffusion are the culprits triggering corrosion reactions and dendrite growth, threatening the sustainability of aqueous zinc‐carbon capacitors. Herein, a polyfunctional biomolecular, vitamin B6, is introduced into the traditional aqueous electrolyte for customizing the functional AEI and fine‐regulating the interfacial coordination environment of zinc ions. Specifically, the preferential anchoring of pyridine nitrogen enables trace vitamin (2.0 g L‐1) to construct a robust AEI and suppress corrosion reactions. The hydroxyl function zone provides high‐octane guidance for zinc‐ion diffusion at the AEI, resulting in flat zinc (002) oriented growth. Consequently, the Zn//Zn symmetrical cell features an ultrahigh cumulative capacity of 4.0 Ah cm‐2 under 34% depth of discharge. The vitamin‐optimized zinc‐carbon capacitor features extended operational lifetimes exceeding 8 months (200 thousand cycles at 5.0 A g‐1), and demonstrates a high areal capacity of averaging 0.68 mAh cm‐2 and exceptional durability over 2000 hours at 1.0 A g‐1 under a high discharge depth of zinc anode (averaging 11.6%). This work offers valuable insights into sustainable and cost‐effective zinc‐carbon capacitors.
π‐Lewis Base Activation of Carbonyls and Hexafluorobenzene
Authors: Mondal Aditesh , Breitwieser Kevin , Danés Sergi , Grünwald Annette , Heinemann Frank W. , Morgenstern Bernd , Müller Frank , Haumann Michael , Schütze Maximilian , Kass Dustin , Ray Kallol , Munz Dominik
Published: December 2024

We report hitherto elusive side‐on η2‐bonded palladium(0) carbonyl (anthraquinone, benzaldehyde) and arene (benzene, hexafluorobenzene) palladium(0) complexes and present the catalytic hydrodefluorination of hexafluorobenzene by cyclohexene. The comparison with respective cyclohexene, pyridine and tetrahydrofuran complexes reveals that the experimental ligand binding strengths follow the order THF<C6H6<C6F6<cyclohexene<pyridine<benzaldehyde<anthraquinone. To understand this surprising order, the complexes’ electronic structures were elucidated by nuclear magnetic resonance (NMR), single crystal X‐Ray diffraction (sc‐XRD), ultraviolet/visible (UV/Vis) electronic absorption, infrared (IR) vibrational, Pd L3‐edge X‐ray absorption (XAS), and X‐ray photoelectron (XP) spectroscopic techniques, complemented by Density Functional Theory (DFT) calculations including energy decomposition (EDA‐NOCV) and effective oxidation state (EOS) analyses. For benzene, pyridine and cyclohexene, bonding follows the donor/acceptor picture of the Dewar–Chatt–Duncanson model. In stark contrast, hexafluorobenzene, benzaldehyde and anthraquinone bind via essentially the π‐channel only and thus as π‐analogues of Z‐acceptor ligands. This contribution elucidates the control of functional‐group selectivity in palladium(0) catalysis and delineates a novel strategy to activate electron‐deficient π‐systems.
Manipulating p‐π Resonance through Methoxy Group Engineering in Covalent Organic Frameworks for an Efficient Photocatalytic Hydrogen Evolution
Authors: Luo Zhipeng , Zhu Shipeng , Xue Huanglan , Yang Wanxiang , Zhang Fengtao , Xu Fei , Lin Wei , Wang Hongqiang , Chen Xiong
Published: December 2024

Kinetic factors frequently emerge as the primary constraints in photocatalysis, exerting a critical influence on the efficacy of polymeric photocatalysts. The diverse conjugation systems within covalent organic frameworks (COFs) can significantly impact photon absorption, energy level structures, charge separation and migration kinetics. Consequently, these limitations often manifest as unsatisfactory kinetic behavior, which adversely affects the photocatalytic activity of COFs. To address these challenges, we propose a methoxy (−OMe) molecular engineering strategy designed to enhance charge carrier kinetics and mitigate mass transfer resistance. Through strategic modulation of the position and quantity of −OMe units, we can effectively manipulate the p‐π conjugation, thereby enhancing charge separation and migration. Moreover, COFs enriched with −OMe moieties exhibit enhanced mass transfer dynamics due to the hydrophilic nature of methoxy groups, which facilitate the diffusion of reactants and products within the porous structure. This approach is hypothesized to drive an efficient photocatalytic hydrogen evolution reaction.
Optimized Adsorption of Had and OHad over Amorphous SrRuPtOxHy Nanobelts towards Efficient Alkaline Fuel Cell Catalysis
Authors: Liu Siyu , Liu Shangheng , Bao Jingliang , Huang Zhongliang , Wei Licheng , Chen Nanjun , Hu Zhiwei , Huang Wei-Hsiang , Pao Chih-Wen , Kong Qingyu , Han Jiajia , Li Leigang , Huang Xiaoqing
Published: December 2024

PtRu‐based catalysts toward hydrogen oxidation reaction (HOR) suffer from low efficiency, CO poisoning and over‐oxidation at high potentials. In this work, an amorphization strategy is adopted for preparation of amorphous SrRuPtOxHy nanobelts (a‐SrRuPtOxHy NBs). The a‐SrRuPtOxHy NBs have optimized adsorption of intermediates (H and OH), increased number of active sites, highly weakened CO poisoning and enhanced anti‐oxidation ability owing to the special amorphous structure. Consequently, a‐SrRuPtOxHy NBs displays superior HOR performance with a mass activity of 7.3 A/mgPt+Ru, 23 and 5 times of that of SrRuPt(OH)x NBs and commercial PtRu/C, respectively, and long‐lasting stability. Besides, a peak power density of 750 mW/cm2 and a specific power of 14.8 W/mgPt+Ru have been achieved for a‐SrRuPtOxHy NBs at a low loading of 0.05 mgPt+Ru/cm2, surpassing many reported HOR catalysts. Mechanism investigation indicates that Pt and Ru are present in oxide/hydroxide forms and H in a‐SrRuPtOxHy NBs participates in HOR. Ab initio molecular dynamics (AIMD) simulations and density functional theory (DFT) calculations show that there are three catalytic mechanisms participating in a‐SrRuPtOxHy NBs, which all exhibit low catalytic barrier and highly improved HOR efficiency. This work provids a new strategy for designing high‐performance catalysts towards fuel cells.