bluuebunny/crossref_metadata_2025 huggingface dataset:
Implementation of the Lupus Low Disease Activity State in Pediatric Rheumatology Care: The Role of the Visual Analog Scale
Authors: Ogbu Ekemini A. , Sagcal‐Gironella Anna Carmela P. , Eberhard B. Anne , Huggins Jennifer M. , Klein‐Gitelman Marisa S. , Onel Karen , Chen Chen , Huang Bin , Brunner Hermine I.
Published: October 2024

Objective

We compared the measurement properties of a traditional physician global assessment of disease activity (PhGA) 10‐cm visual analog scale (PhGA0–10) with that of the three‐point numeric scale (PhGA0–3) in childhood‐onset systemic lupus erythematosus (cSLE) as part of the childhood Lupus Low Disease Activity State (cLLDAS).

Methods

We used a secondary data analysis from a convenience sample of 100 patients with cSLE followed every three months for up to seven visits. Ratings of PhGA0–10, PhGA0–3, parent assessment of patient well‐being (ParGA) (range: 0= very poorly, 10 = very well), disease activity as measured by the SLE disease activity index 2000 (SLEDAI‐2k), Safety of Estrogens in Lupus Erythematosus National Assessment (SELENA) SLEDAI, and the British Isles International Lupus Activity Group index (BILAG; A = 9, B = 3, C = 1, D/E = 0) were compared. After linear transformation of PhGA0–10 to a 0 to 3 range (tPhGA0–10), the frequency of PhGA0–3 ≤1 was assessed to estimate the impact of scale type on the scoring of the cLLDAS.

Results

In 600 visits, the median (range) scores of PhGA0–10, PhGA0–3, SLEDAI‐2k, SELENA‐SLEDAI, and BILAG were 2 (0–10), 1(0–3), 4 (0–28), 4 (0–32), and 2 (0–28), respectively. PhGA0–10 and PhGA0–3 ratings were strong to moderately correlated with (r = 0.73; P < 0.0001) and with more variability for PhGA0–3 ≥2. SELENA‐SLEDAI and SLEDAI‐2k scores were moderately correlated with PhGA0–10 (r = 0.56/0.54; P < 0.0001). ParGA values were weakly correlated with all other measures considered (all r = −0.19 to −0.34). There were 490 of 600 visits with PhGA0−3 ≤1 and 497 of 600 visits with tPhGA0−10 ≤1 (κ (SE) =0.59 (0.04), McNemar P = 0.4).

Conclusion

PhGA0–3 and PhGA0–10 have comparable measurement properties and yield almost identical cLLDAS rates when used in cSLE.
The Energy Absorption Characteristics and Sound Absorption Behavior of In Situ Integrated Aluminum Lattice Structure Filled Tubes
Authors: Wang Han , Wang Kedi , Ma Pengwei , Fan Xueling
Published: October 2024

Lattice structures, as integrated structure‐function engineering materials, have developed rapidly in industrial fields. In this study, the in situ integrated solid/hollow aluminum lattice structure filled tubes are designed and manufactured by a selective laser melting technique. The effects of structure parameters on compressive properties, energy absorption, and sound absorption are analyzed. The in situ integrated aluminum lattice structure filled tubes with hollow lattice structure and strengthened hollow lattice structure can achieve a wide adjustment of compressive property (31.04–185.64 MPa) and energy absorption density (11.21–51.70 MJ m−3) in a narrow density range. The compressive property and energy absorption are superior compared with ex situ aluminum lattice structure filled tubes due to the interaction and metallurgical bonding between the thin‐walled tubes and the aluminum lattice structures. The hollow structure design and altering its structure parameters can regulate the sound absorption coefficient and the corresponding peak frequency (the highest absorption peak is 0.723 at 2098 Hz). In addition, the hollow structure design can realize double absorption peaks (0.360 at 1462 Hz and 0.503 at 2122 Hz), presenting the potential for broadband sound absorption. Eventually, superior integrated energy/sound absorption structures can be obtained by the hollow structure design and its corresponding optimization.
Heterostructure Engineering of Biphase‐Coupled Ternary Transition Metal Phosphoselenide by Topological Transformation Enabling High Performance for Supercapacitors
Authors: Zhao Liyun , Li Yanyan , Zhao Jiayang , Zhang Haotian , Yuan Pengfei , Song Rui
Published: October 2024

The exploration of promising electrode materials with structural stability and rapid interfacial reaction kinetics is highly desirable for supercapacitors toward large‐scale applications. Herein, the synthesis of biphase‐coupled CoPSe/NiP0.24Se1.76 with multiple in‐plane heterointerfaces using the in situ topological transformation approach is presented. As a novel ternary metal phosphoselenide (TMPSe) for supercapacitor cathode that is fabricated by synchronous phosphoselenization strategy, it realizes a superior lifespan with cycling compared to conventional transition metal selenides. The depleted anti‐bonding eg* orbitals of transition metal ions (Co/Ni) in the CoPSe/NiP0.24Se1.76, as proved by preliminary theoretical calculations, strengthens the chemical bonding between Co/Ni and coordinating atoms, thereby enhancing the chemical stability. Simultaneously, the CoPSe/NiP0.24Se1.76 in‐plane multi‐heterostructures can not only alleviate the volume change during the charge–discharge process but also expose more active sites, promoting the adsorption of OH− ions, which is conducive to the rapid redox reaction kinetics of the CoPSe/NiP0.24Se1.76, and consequently, it delivers a remarkable reversible capacity and excellent long‐term cycle stability with 97.7% initial capacitance retention over 16 000 cycles. Moreover, the asymmetric supercapacitors with this cathode demonstrate outstanding rate capability and high energy density. This strategy of constructing biphase‐coupled CoPSe/NiP0.24Se1.76 by topological transformation is of great potential application for the high‐performance electrode material.
Anchoring Ag Atom on Carbon Vacancy Enriched Carbon Nitride to Synergistically Promote CO2 Photoredution with Water
Authors: Zhang Yu , Zhai Mianmian , Liu Juan , Xu Jixiang , Lin Haifeng , Xing Jun , Wang Lei
Published: October 2024

Pristine carbon nitride (CN) has low CO2 reduction ability due to its sluggish charge carriers transfer and CO2 activation. Herein, carbon vacancy (CV) and Ag single atoms (SAs) with N2 coordination are simultaneously introduced into CN with the ordered structure for stable and efficient photoreduction of CO2 in the presence of H2O. The optimal sample loaded with 0.053 wt.% Ag evolve 173.0 µmol g−1 CO in 3 h with 89% selectivity, which is 11.7 times higher than that of pristine CN (14.7 µmol g−1). Experiments and theoretical calculations reveal that the CV and Ag–N2 sites promote CO2 adsorption/activation and the generation of *COOH and *CO. KSCN‐assisted calcination induces more ordered arrangement of melon chains, which can accelerate charge transfer/separation and facilitate H2O oxidation, thus accounting for the largely improved CO2 photoreduction performance. This study adopts a new method to prepare Ag SA‐anchored and C‐deficient CN, and provides insights into their synergistic roles in enhancing CO2 reduction.
Spatial‐Dependent Coupling of Electrochemistry, Mass Transport, and Stress in Silicon‐Graphite Composite Electrodes for Lithium‐Ion Batteries
Authors: Li Xueyan , Chen Yongtang , Lu Yuyang , Fu Kang , He Xingmin , Sun Kai , Ding Junjie , Ni Yong , Tan Peng
Published: October 2024

The commercialization of high‐capacity silicon materials in lithium‐ion batteries is hindered by significant volume changes. Composite anodes made from silicon and graphite, which increase battery capacity and maintain electrode structural stability, are receiving considerable attention. However, the spatial configuration of the active particles in the electrode is few investigated due to the complexity of experiments at the microscopic scale. Herein, this work focuses on electrochemical, mass transport, and stress coupling mechanisms by considering different spatial configurations of silicon and graphite. In situ electrochemical and stress measurements are first conducted to demonstrate the impact of the active material arrangement. Then, a 2D electrochemical‐mechanical model is developed considering the heterogeneity of electrochemical processes at the particle‐electrolyte interface. The results show that placing silicon in the upper active layer significantly reduces the ion transport resistance, while the graphite layer near the current collector provides a good conductive network for electron transport in the silicon layer, enhancing the performance of the composite electrode structure. By combining electrochemical and mechanical field models with experimental verification, this study deepens the understanding of composite electrode structure design, offering practical guidance for optimizing the spatial configuration of electrode materials to significantly improve battery performance.
Biodegradable Citrate‐Based Polymers Enable 5D Monitoring of Implant Evolution
Authors: Shan Dingying , Wang Dingbowen , Ma Yuncong , Liang Zhifeng , Ravnic Dino J. , Zhang Nanying , Yang Jian
Published: October 2024

Biodegradable tissue engineering scaffolds have garnered increasing interest for their role in providing mechanical support, promoting tissue regeneration, and eliminating the need for removal. However, the in vivo degradation processes remain challenging to track. Here, a novel biodegradable polymer, N‐methyldiethanolamine (MDEA) and Gadolinium(III) diethylenetriamine pentaacetate (Gd‐DTPA) modified biodegradable photoluminescent polymers (BPLPMGd), which combines near‐infrared (NIR) fluorescence and magnetic resonance (MR) dual‐modality imaging are introduced to monitor scaffold degradation in vivo. The chemical structure of BPLPMGd is characterized and its dual‐imaging properties in vitro are evaluated. Subsequently, non‐invasive dual‐modality imaging to track the degradation of implanted BPLPMGd scaffolds is performed in a rat model, comparing these results with histological data. This approach reveals that BPLPMGd enables reliable non‐invasive tracking of the degradation, where NIR fluorescence imaging offers a qualitative and quantitative analysis of scaffold mass loss, total volume and solid content changes, while magnetic resonance imaging (MRI) details structural and morphological changes, allowing for 5D monitoring of implant degradation, including 3D structure, location, mass, volume, and geometry. The combination of these imaging modalities provides a comprehensive view of scaffold degradation, where the synergistic use of both yields results greater than either modality alone, offering unprecedented 5D information of implantable devices. This innovative approach has potential applications in regenerative engineering and beyond.
Wearable Haptics for Orthotropic Actuation Based on Perpendicularly Nested Auxetic SMA Knotting
Authors: Khan Mannan , Oh Saewoong , Song Tae‐Eun , Ji Wonhee , Mahato Manmatha , Yang Yang , Saatchi Daniel , Ali Syed Sheraz , Roh Jaewoo , Yun Donghyeok , Ryu Jee‐Hwan , Oh Il‐Kwon
Published: October 2024

Smart wearable tactile systems, designed to deliver different types of touch feedback on human skin, can significantly improve engagement through diverse actuation patterns in virtual or augmented reality environments. Here, a perpendicularly nested auxetic wearable haptic interface is reported for orthotropically decoupled multimodal actuation (WHOA), capable of producing diverse tactile feedback modes with 3D sensory perception. WHOA incorporates shape memory alloy wires that are intricately knotted into an auxetic structure oriented along orthotropic dual axes. Its perpendicularly nested auxetic structure enables orthotropic actuation, allowing independent expansion and contraction along both x and y‐axes, as confirmed by force‐strain and displacement‐time performance tests. Additionally, the perylene coating provides orthogonal electrical isolation to WHOA, allowing for stripe‐specific localized actuation and enabling multiple tactile feedback modes. As an orthotropic wearable haptic interface, WHOA distinguishes between x‐axis and y‐axis directions and ultimately delivers multi‐dimensional information regarding movements in 3D space through tactile feedback. As a result, when worn on the foot or arm, WHOA naturally delivers spatiotemporal tactile information to the user, facilitating navigation and teleoperation with 3D sensory perception.
Recent Advances in High‐Entropy Layered Oxide Cathode Materials for Alkali Metal‐Ion Batteries
Authors: Duan Liping , Zhang Yingna , Tang Haowei , Liao Jiaying , Zhou Guangmin , Zhou Xiaosi
Published: October 2024

Since the electrochemical de/intercalation behavior is first detected in 1980, layered oxides have become the most promising cathode material for alkali metal‐ion batteries (Li+/Na+/K+; AMIBs) owing to their facile synthesis and excellent theoretical capacities. However, the inherent drawbacks of unstable structural evolution and sluggish diffusion kinetics deteriorate their electrochemical performance, limiting further large‐scale applications. To solve these issues, the novel and promising strategy of high entropy has been widely applied to layered oxide cathodes for AMIBs in recent years. Through multielement synergy and entropy stabilization effects, high‐entropy layered oxides (HELOs) can achieve adjustable activity and enhanced stability. Herein, the basic concepts, design principles, and synthesis methods of HELO cathodes are introduced systematically. Notably, it explores in detail the improvements of the high‐entropy strategy on the limitations of layered oxides, highlighting the latest advances in high‐entropy layered cathode materials in the field of AMIBs. In addition, it introduces advanced characterization and theoretical calculations for HELOs and proposes potential future research directions and optimization strategies, providing inspiration for researchers to develop advanced HELO cathode materials in the areas of energy storage and conversion.
Trifluoroacetic Acid Promotes Umpolung of 2‐Methylindole to Achieve C(sp3)−H Activation
Authors: Kong Hongmei , Li Kuo , Zhang Jingfa , Yan Hua , Jing Lisha , Liu Yuyin , Song Chenggang , Zhou Pan , Wang Bin
Published: October 2024

An umpolung strategy for the C(sp3)−H aminomethylation of 2‐methylindole has been developed using trifluoroacetic acid to induce the transformation, with aminals serving as precursors of iminium ion. Mechanistic studies have clearly shown that trifluoroacetic acid may play a pivotal role in this strategy. The utilization of readily available starting materials, mild reaction conditions, tolerance to complex functional groups, combine with yields of up to 98% and potential biological applications render this protocol applicable and useful for organic synthesis and medicinal chemistry.
Robust Whole‐Cell‐Based Chemoenzymatic Synthesis of Site‐Selective Deuterated α‐Hydroxy Acids and α‐Amino Acids
Authors: Yu Keying , Liu Yanqiong , Zhang Jingxuan , Zhao Wushuang , Mao Yingle , Liao Cangsong
Published: October 2024

Deuterated hydroxyl acids and amino acids have been widely utilized in life science, biochemistry and drug development. Site‐selective and stereoselective synthesis of deuterated hydroxyl acids and amino acids remains a significant challenge. Here, we report the development of a robust whole‐cell‐based chemoenzymatic platform for the synthesis of deuterated hydroxyl acids and amino acids from off‐the‐shelf aldehydes in high yields with excellent selectivities and levels of deuteration. The platform delivers products with diverse scaffolds and deuteration patterns, as well as broad scopes with both aromatic and aliphatic side chains. The application of the platform was demonstrated by the concise synthesis of a deuterium‐containing antiparkinson's disease candidate. This platform provides a concrete foundation for accessing amino acid isotopologs for potential applications in research and drug discovery and development.
Dual Electric‐Double‐Layer Model for Work Function Reduction by Polyethyleneimine Coated on Zinc Oxide: All‐Atom Molecular Dynamics Simulations
Authors: Suzuki Rikuo , De Nicola Antonio , Kido Junji , Matsui Hiroyuki , Milano Giuseppe
Published: October 2024

Polyethyleneimine (PEI) can reduce work function when applied to cathode surface and to improve the drive efficiency of various organic electronic devices. Clarifying the mechanism of the work function reduction is important in developing alternative materials with higher stability. In this paper, a PEI thin film coated on a ZnO layer using all‐atom molecular dynamics simulations is analyzed. The simulations show that the entire PEI thin film induces an electrostatic potential shift of 0.30 eV, whose magnitude and sign are in good agreement with experiments. Further analysis reveals that there are two electric double layers (EDLs) at the ZnO/PEI interface and PEI/vacuum surface and that the latter plays a major role. The coil‐shell conformation of PEI at the PEI/vacuum surface forms the outer EDL and reduces the work function. At the ZnO/PEI interface, on the other hand, the coil‐shell conformation is less dominant because of the Zn‐N interaction and the inner EDL causes a small increase of the work function. This dual EDL model is different from the single EDL model for self‐assembled monolayers in that polymer conformations are essential. The report clarifies the novel polymer‐specific mechanism of work function reduction and opens up the possibility of new cathode modifiers.
Humoral Immunity Profiling to Pandemic and Bat‐Derived Coronavirus Variants: A Geographical Comparison
Authors: Fathi Parinaz , Alfonso Andrea Lucia , Yek Christina , Putman Zoe , Drew Matthew , Esposito Dominic , Zaidi Irfan , Chea Sophana , Ly Sokna , Sath Rathanak , Lon Chanthap , Chea Huch , Leang Rithea , Huy Rekol , Ly Sovann , Seng Heng , Tan Chee Wah , Zhu Feng , Wang Lin‐Fa , Oliveira Fabiano , Sadtler Kaitlyn , Manning Jessica
Published: October 2024

Dynamic pathogen exposure may impact the immunological response to SARS‐CoV‐2 (SCV2). One potential explanation for the lack of severe SCV2‐related morbidity and mortality in Southeast Asia is prior exposure to related betacoronaviruses. Recent discoveries of SCV2‐related betacoronaviruses from horseshoe bats (Rhinolophus sinicus) in Thailand, Laos, and Cambodia suggest the potential for bat‐to‐human spillover exposures in the region. In this work, serum antibodies to protein constructs from SCV2 and a representative bat coronavirus isolated in Cambodia (RshSTT182) are measured in pre‐pandemic Cambodian human sera using ELISA assays. Of 293 Cambodian samples tested (N = 131 with acute malaria, n = 162 with acute undifferentiated febrile illness), 32 (10.9%) are seropositive for SCV2 based on established Spike and receptor‐binding domain (RBD) cutoffs. Within SCV2 seropositive samples, 16 (50%) have higher antibody levels to antigens from the representative virus RshSTT182 versus SCV2 antigens; competitive binding ELISA assays demonstrate inhibition of reactivity to SCV2 Spike after pre‐incubation with RshSTT182 Spike. Surrogate virus neutralization tests demonstrate that 8/30 (26.7%) SCV2 ELISA positive pre‐pandemic Cambodian samples have neutralizing activity against SCV2, while 14/30 (46.7%) have activity against other SCV2‐related betacoronaviruses. These data suggest that exposure to related betacoronaviruses may elicit cross‐reactive immunity to SCV2 prior to the global pandemic.
LncRNA evf‐2 Exacerbates Podocyte Injury in Diabetic Nephropathy by Inducing Cell Cycle Re‐entry and Inflammation Through Distinct Mechanisms Triggered by hnRNPU
Authors: Zhang Chaojie , Zhao Hui , Yan Yufan , Li Yanfei , Lei Min , Liu Yong , Yang Longhua , Zhao Huijian , Zhou Sijie , Pan Shaokang , Liu Zhangsuo , Guo Jia
Published: October 2024

Albuminuria is a hallmark of diabetic nephropathy (DN). Podocyte injury significantly contributes to proteinuria in DN. Our study found that lncRNA EVF‐2 is upregulated in podocytes of DN patients, correlating with cell cycle re‐entry and inflammation. Specific knockout or knockdown of lncRNA evf‐2 in diabetic mice or cultured podocytes alleviated podocyte injury associated with these processes. RNA sequencing of evf‐2‐overexpressing podocytes unveiled a predominant enrichment of upregulated mRNAs in cell cycle and inflammation pathways, with alternative splicing in cell cycle‐related mRNAs Ccnb1 and Tacc3. Chromatin isolation by RNA purification‐mass spectrometry (ChIRP‐MS) analysis highlighted the involvement of ribonucleoprotein complex and mRNA processing‐related proteins, with hnRNPU as the main binding partner of evf‐2 in spliceosomes. Knockdown of hnRNPU partially restored the upregulation of mRNAs induced by evf‐2 overexpression, altering splice variants of Ccnb1 and Tacc3. This study is the first to reveal the splice variants of cell cycle‐related genes in DN and elucidate the interaction between lncRNA evf‐2 and hnRNPU. This interaction culminates in the upregulation of cell cycle‐related genes and inflammatory factors through diverse pathways, potentially involving transcriptional activation, RNA stability modulation, alternative splicing or translational regulation. This highlights potential novel pathways for DN treatment.
Nuclear Decommissioning and Sustainable Environment: Insights on Decontamination Processes
Authors: Ngulimi Miguta Faustine , Kim Sion , Asghar Kamal , Seo Bum Kyoung , Roh Changhyun
Published: October 2024

Nuclear energy accounts for ≈10% of global energy production, positioning it as a promising solution for achieving carbon neutrality amid escalating concerns over climate change. Nonetheless, the effective management of radioactive waste, which can remain hazardous for up to one hundred thousand years, presents considerable challenges that must be addressed to uphold public trust and safeguard environmental safety. This review outlines the fundamental stages of nuclear decommissioning including strategic planning, decontamination, dismantling, remediation, encapsulation, deregulation, and site reuse as a critical component of sustainable environmental practices. The review also highlights the significance of efficient decontamination processes in reducing waste generation. Various decontamination techniques, including mechanical, electromechanical, chemical, and advanced methods such as laser and plasma decontamination, are evaluated for their effectiveness and limitations. Moreover, the review emphasizes the need to enhance the recovery and recycling of ion exchange resin and potential radionuclides during decontamination processes to minimize waste and to address the depletion of potential radionuclide resources. Future research should prioritize the development of innovative techniques for decontamination and radioactive waste management, fostering sustainable decommissioning and supporting the ongoing development of nuclear energy in an environmentally responsible manner.
A Star‐Nose‐Inspired Bionic Soft Robot for Nonvisual Spatial Detection and Reconstruction
Authors: Shan Qiwei , Cao Yunqi , Chi Haozhen , Fan Shuyu , Zhu Ziying , Hou Dibo
Published: October 2024

The star‐nosed mole is recognized as a tactilely sensitive mammal due to its unique nose, which facilitates spatial detection in dark environments through touch using its appendages enveloped in numerous sensory receptors. This article introduces a bionic soft robot inspired by the star‐nosed mole, which combines a pneumatic soft platform with a polydimethylsiloxane–polyethylene terephthalate cylindrical tactile sensor array based on bilayer single‐electrode triboelectric nanogenerators, mimicking the muscle tissue of the mole's nose and the cylindrical appendages surrounded by Eimer's organs. The cylindrical sensor array enables multiangle spatial detection without an external power supply and remains unaffected by external materials. By implementing a constant curvature model for robot motion control, positional information is provided for the contact points between the cylindrical sensor array and the external environment. The robot effectively discriminates the distance and shape of various objects and achieves nonvisual 3D spatial detection and reconstruction in real‐world scenarios. This work presents a novel bionic approach for 3D spatial detection in nonvisual environments.
Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin
Authors: Anderson Ian C. , Gomez Darwin C. , Zhang Meijing , Koehler Stephen J. , Figg C. Adrian
Published: October 2024

Protein photocatalysts provide a modular platform to access new reaction pathways and affect product outcomes, but their use in polymer synthesis is limited because co‐catalysts and/or co‐reductants are required to complete catalytic cycles. Herein, we report using zinc myoglobin (ZnMb), an inherently photoactive protein, to mediate photoinduced electron/energy transfer (PET) reversible addition‐fragmentation chain transfer (RAFT) polymerizations. Using ZnMb as the sole reagent for catalysis, photomediated polymerizations of N,N‐dimethylacrylamide in PBS were achieved with predictable molecular weights, dispersity values approaching 1.1, and high chain‐end fidelity. We found that initial apparent rate constants of polymerization increased from 4.6×10–5 s−1 for zinc mesoporpyhrin IX (ZnMIX) to 6.5×10–5 s−1 when ZnMIX was incorporated into myoglobin to yield ZnMb, indicating that the protein binding site enhanced catalytic activity. Chain extension reactions comparing ZnMb‐mediated RAFT polymerizations to thermally‐initiated RAFT polymerizations showed minimal differences in block copolymer molecular weights and dispersities. This work enables studies to elucidate how protein modifications (e.g., secondary structure folding, site‐directed mutagenesis, directed evolution) can be used to modulate polymerization outcomes (e.g., selective monomer additions towards sequence control, tacticity control, molar mass distributions).
Catalytic Enantioselective Synthesis of Boron‐Stereogenic and Axially Chiral BODIPYs via Rhodium(II)‐Catalyzed C−H (Hetero) Arylation with Diazonaphthoquinones and Diazoindenines
Authors: Gao Yankun , Liu Zizhen , Tian Sichao , Min Ying , Li Xiangyu , Chen Yuxi , Hong Xin , Zhang Weidong , Wang Lei
Published: October 2024

The molecular engineering of boron dipyrromethenes (BODIPYs) has garnered widespread attention due to their structural diversity enabling tailored physicochemical properties for optimal applications. However, catalytic enantioselective synthesis of structurally diverse boron‐stereogenic BODIPYs through intermolecular desymmetrization and BODIPYs with atroposelectivity remains elusive. Here, we showcase rhodium(II)‐catalyzed site‐specific C−H (hetero)arylations of prochiral BODIPYs and polysubstituted BODIPYs with diazonaphthoquinonesand diazoindenines, providing efficient pathways for the rapid assembly of versatile (hetero)arylated boron‐stereogenic and axially chiral BODIPYs through long‐range desymmetrization and axial rotational restriction modes. The synthetic application of the procedures has been emphasized by the efficient synthesis of BODIPY derivatives with various functions. Photophysical properties, bioimaging, and lipid droplet‐specific targeting capability of tailored BODIPYs are also demonstrated, indicating their promising applications in biomedical research, medicinal chemistry, and material science.
Efficient Energy Transfer from Quantum Dots to Closely‐Bound Dye Molecules without Spectral Overlap
Authors: Kurashvili Mariam , Llusar Jordi , Stickel Lena S. , Würthner Tim , Ederle David , Infante Ivan , Feldmann Jochen , Akkerman Quinten A.
Published: October 2024

Quantum dots (QDs) are semiconductor nanocrystals whose optical properties can be tuned by altering their size. By combining QDs with dyes we can make hybrid QD‐dye systems exhibiting energy transfer (ET) between QDs and dyes, which is important in sensing and lighting applications. In conventional QDs that need a shell to passivate surface defects, ET usually proceeds through Förster resonance energy transfer (FRET) that requires significant spectral overlap between QD emission and dye absorbance, as well as large oscillator strengths of those transitions. This considerably limits the choice of dyes. In contrast, perovskite QDs do not require passivating shells for bright emission, which makes ET mechanisms beyond FRET accessible. This work explores the design of a CsPbBr3 QD‐dye system to achieve efficient ET from CsPbBr3 QDs to dyes with dimethyl iminium binding groups where the close binding of dyes to CsPbBr3 surface facilitates spatial wavefunction overlap. Using steady‐state and time‐resolved photoluminescence experiments, we demonstrate that efficient ET from CsPbBr3 to dyes with minimal spectral overlap proceeds via the Dexter exchange‐type mechanism, which overcomes the conventional restriction of spectral overlap that severely limits the tunability of these systems. This approach opens new avenues for QD‐molecule hybrids for a wide range of applications, such as lighting.
The Swiss Army Knife of Electrodes: Pillar[6]arene‐Modified Electrodes for Molecular Electrocatalysis Over a Wide pH Range
Authors: Roithmeyer Helena , Bühler Jan , Blacque Olivier , Tuncay Isik , Moehl Thomas , Invernizzi Cristiano , Keller Florian , Iannuzzi Marcella , Tilley S. David
Published: October 2024

Molecularly‐modified electrode materials that maintain stability over a broad pH range are rare. Typically, each electrochemical transformation necessitates a specifically tuned system to achieve strong binding and high activity of the catalyst. Here, we report the functionalisation of mesoporous indium tin oxide (mITO) electrodes with the macrocyclic host molecule pillar[6]arene (PA[6]). These electrodes are stable within the pH range of 2.4–10.8 and can be equipped with electrochemically active ruthenium complexes through host–guest interactions to perform various oxidation reactions. Benzyl alcohol oxidation serves as a model reaction in acidic media, while ammonia oxidation is conducted to assess the systems performance under basic conditions. PA[6]‐modified electrodes demonstrate catalytic activity for both reactions when complexed to different guest molecules and can be reused by reabsorption of the catalyst after its degradation. Furthermore, the system can be employed to perform subsequent reactions in electrolyte with varying pH, enabling the same electrode to be utilised in multiple different electrocatalytic reactions.
Machine Learning‐Guided Discovery of Copper(I)‐Iodide Cluster Scintillators for Efficient X‐ray Luminescence Imaging
Authors: Wang Yanze , Zhang Tinghao , Zhao Wenjing , Xu Weidong , Wu Zhongbin , Suh Yung Doug , Zhang Yuezhou , Liu Xiaowang , Huang Wei
Published: October 2024

Developing efficient scintillators with environmentally friendly compositions, adaptable band gaps, and robust chemical stability is crucial for modern X‐ray radiography. While copper(I)‐iodide cluster crystals show promise, the vast design space of inorganic cores and organic ligands poses challenges for conventional approaches. In this study, we present machine learning‐guided discovery of copper(I)‐iodide cluster scintillators for efficient X‐ray luminescence imaging. Our findings reveal that combining base learning models with fused features enhances model generalization, achieving an impressive determination coefficient of 0.88. By leveraging this approach, we obtain a high‐performance Cu(I)‐I cluster scintillator, named copper iodide‐(1‐Butyl‐1,4‐diazabicyclo[2.2.2]octan‐1‐ium)2, which exhibit radioluminescence 56 times stronger than that of PbWO4, and enables a detection limit for X‐rays of 19.6 nGyair s−1. Furthermore, we demonstrate the versatility of these scintillators by incorporating them as microfillers in the fabrication of flexible composite scintillators for X‐ray imaging, achieving a static resolution of 20 lp mm−1 and demonstrating promising performance for dynamic X‐ray imaging.
Suppression of Structural Heterogeneity in High‐Entropy Intermetallics for Electrocatalytic Upgrading of Waste Plastics
Authors: Hao Jiace , Wang Tongde , Cai Jian , Gao Guohua , Zhuang Zechao , Yu Ruohan , Wu Jinsong , Wu Guangming , Lu Shuanglong , Wang Xiaofan , Du Mingliang , Wang Dingsheng , Zhu Han
Published: October 2024

The key to fully realizing the potential of high‐entropy alloys (HEAs) lies in balancing their inherent local chemical disordering with the long‐range ordering required for electrochemical applications. Herein, we synthesized a distinctive L10‐(PtIr)(FeMoBi) high‐entropy intermetallics (HEIs) exhibiting nanoscale long‐range order and atomic scale short‐range disorder via a lattice compensation strategy to mitigate the entropy reduction tendency. The (PtIr)(FeMoBi) catalyst exhibited remarkable activity and selectivity of glycollic acid (GA) production via electrocatalytic waste polymer‐derived ethylene glycol oxidation reaction (EGOR). With a mass activity of 5.2 A mgPt−1 and a Faradaic efficiency (FE) for GA of 95 %, it outperformed most previously reported electrocatalysts for selective GA production. The lattice‐compensation effect promotes the homogeneity of Pt and Fe actives sites, facilitating co‐adsorption of EG and OH and reducing the energy barriers for dehydrogenation and OH‐combination processes. This approach effectively avoids the formation of low‐active sites commonly encountered in HEA solid solutions, offering a promising avenue for exploring the complex interplay between catalytic activity and HEI structures.
Reductive C(sp2)−Si Cross‐Couplings by Catalytic Sodium‐Bromine Exchange
Authors: Neil Baptiste , Deis Thomas , Fensterbank Louis , Chauvier Clément
Published: October 2024

The metal‐halogen exchange reaction constitutes one of the most important preparative routes towards polar organometallic reagents such as aryllithium or Grignard reagents. However, despite extensive developments over the past eight decades, this fundamental organometallic elementary step has only been exploited stoichiometrically. Against this background, we demonstrate that the sodium‐bromine exchange reaction can be implemented in a catalytic setting as a mean to activate C(sp2)−Br bonds in a transition metal‐free manner en route to the regioselective and general preparation of (hetero)aryl silanes. Simply treating structurally diverse (hetero)aryl bromides with N‐tert‐butyl‐N’‐silyldiazenes (tBu−N=N−Si) as silylating reagents and inexpensive sodium alkoxides as catalytic promoters yields a range of aromatic organosilicon compounds under ambient conditions. Mechanistic studies provide solid evidence for the involvement of tert‐butyl sodium as the C(sp2)−Br metalating agent.
Bioactivity Modulation: Anionic Influence on Cu(II) Schiff Base Complexes
Authors: Sebastian Jesna K. , Amrutha S. R. , Suja N. R. , Mohan Nithya , Sreejith S. S. , Sithambaresan Maheswaran , Priya M. , Muraleedharan Nair M. K.
Published: October 2024

This article explains the synthesis of three Schiff base Cu(II) complexes derived from 3‐hydroxybenzaldehyde and ethylenediamine using three distinct copper anionic salts, and it explores the effects of those salts on the properties of the complexes. Elemental analysis, electronic spectra, FT‐IR, ESR, molar conductance, magnetic measurement, thermogravimetric analysis and PXRD were used to characterize the compounds. The anionic salt has been demonstrated to exhibit distinctive characteristics on Gram‐positive and Gram‐negative bacteria in terms of structure, DNA binding, cell viability, DNA breakage and activity. Furthermore, this ligand L1 and its derivatives indicated positive antifungal efficacy against Aspergillus niger and Trichophyton tonsurans. The study elucidates the manner in which distinct anion salts impacted the properties of complexes and their antifungal, anticancer and antibacterial outcomes.
Electron‐Deficient Indenofluorene‐Based Systems: Multicolor and Visible‐To‐Near‐Infrared (NIR) Electrochromism and OFF‐OFF‐ON Electrofluorochromism
Authors: Nipate Atul B. , Kamble Abhijeet V. , Rao M. Rajeswara
Published: October 2024

Multifunctional electrochromic systems with divergent functions are highly sought after but rare and challenging to develop. Here, we report the synthesis and multi‐functional electrochromic behaviour (multi‐colour modulation, visible‐to‐near IR absorption switching, and electrofluorochromism) of electron‐deficient indenofluorene‐based systems. The compounds (IF1‐IF5) have been obtained via Knoevenagel condensation of indenofluorenone (IFK) with various nucleophiles (malononitrile, benzylcyanide, dimethyl malonate, methyl cyanoacetate, benzothiazole‐2‐acetonitrile). IF1‐IF5 possess strong colours and absorb in the visible region (λmax=295–388 nm). These compounds are electroactive and exhibit two reversible reduction waves (−0.35–−0.88 V and −0.65–−1.30 V vs Ag/AgCl), generating radical anion and dianion systems. For the electrochromic studies, upon applying the one‐electron reduction potential (−0.35 V vs Ag/AgCl), the absorption maximum of IF1 redshift from 382 nm to 1240 nm (IF1−⋅), which subsequently blueshifts to 466 & 745 nm (IF12−⋅) upon increasing to two‐electron reduction potential (−0.65 V vs Ag/AgCl). The color of the solution was switched from green to dark blue and further to light orange. The electrochromic behaviour is highly reversible and cycling. In addition, unlike the non‐fluorescent (IF1 and IF1−⋅), the two‐electron reduced system (IF12−⋅) is red‐emissive (λem=630 nm) due to the combination of radicals leading to the formation of antiaromatic quinoidal π‐conjugated system (IF12−).
Visible Light‐Driven Metal‐ and Photocatalyst‐Free Synthesis of β‐Trifluoromethylated Enamines via Trifluoromethyl Thianthrenium Salts
Authors: Jiang Liang , Tang Yisong , Li Shaxuan , Peng Xing , Saffar Andaloussi Rim , Chen Xiao Yun
Published: October 2024

A novel protocol for the visible‐light‐driven synthesis of β‐trifluoromethylated enamines has been developed, which operates without the use of transition metals or any photocatalysts, utilizing trifluoromethylthiosulfonium salts as the source of trifluoromethyl groups under mild conditions. According to this new protocol, more than 40 products have been prepared in moderate to good yields. In addition to eliminating the need for expensive or toxic transition metals and photocatalysts, this new methodology proves its potential scalability through air‐stability, the use of safe and readily available reagents, a two‐step one‐pot procedure, and effective gram‐scale reactions. This innovative approach not only demonstrates promise for green chemical synthesis but also offers a new pathway for the advancement of fluorine chemistry in sustainable organic synthesis.
Stability analysis of aperiodic impulsive delay systems using sum of squares approach
Authors: Qi Jiangtao , Sun Yanhan
Published: October 2024

The stability problem of aperiodic impulsive delay systems with unstable continuous and discrete dynamics is addressed in this article. New delay‐dependent stability conditions are proposed by employing a clock‐dependent Lyapunov–Krasovskii‐like functional composed of a Lyapunov–Krasovskii functional and a high‐order polynomial matrix function. The stability conditions are then solved using sum of squares programming techniques, yielding less conservative results than the looped‐functionals approach. Finally, the simulation results demonstrate the effectiveness of the results.
Combined Impedance and Electron Paramagnetic Resonance Spectroscopy for Investigating the Dynamics of Li/Solid Li‐ion Conductor Interfaces
Authors: Götz Rainer , Wagner Michael , Song Kun‐Ting , Katzenmeier Leon , Bandarenka Aliaksandr S.
Published: October 2024

Electrochemical impedance spectroscopy (EIS) is a widely used tool for the electrochemical characterization of all‐solid‐state batteries (ASSBs) with Li‐metal anodes. However, an unambiguous interpretation of the observed impedance response often requires additional independent information on the actual interfacial phenomena obtained. The measurement methodology presented in this study allows to conduct electron paramagnetic resonance (EPR) spectroscopy and EIS concurrently. Therefore, the informative power of EIS experiments can be significantly improved via monitoring of structural changes of paramagnetic lithium at the electrochemical interface. As the solid‐electrolyte‐lithium interface is a critical part of all‐solid‐state batteries, this study employs a model oxide solid electrolyte in contact with lithium metal. During the polarization of the cell with thin evaporated lithium electrodes, the ratio between positive and negative peaks (a/b) of the EPR signal momentarily rises, which indicates an accumulation of lithium on one side of the electrolyte. The peak ratio a/b then drops abruptly, accompanied by current irregularities. Both are indicative of a diminishing contact area, and as a result, finer lithium morphologies form. Shortly after that, a contact loss is observed. The change of the EPR signal shape before cell breakdown can hence be associated with the worsening Li‐electrolyte contact, providing a tool for physical in‐situ cell diagnostics.
3D Printable Alginate–Chitosan Hydrogel Loaded With Ketoconazole Exhibits Anticryptococcal Activity
Authors: Mace Manoela Almeida Martins , Reginatto Camila Leites , Silva Victória Rapack Jacinto , Pinheiro Ana Carolina Silva , Silva Laiane Souza da , Moura Dinara Jaqueline , Fuentefria Alexandre Meneghello , Soares Rosane Michele Duarte
Published: October 2024

Natural polymers have recently been investigated for various applications, such as 3D printing and healthcare, including treating infections. Among microbial infections, fungal diseases remain overlooked, with limited therapeutic options and high recurrence. Cutaneous cryptococcosis is an opportunistic fungal infection triggered by mechanical inoculation or hematogenous dissemination of the yeast that causes cryptococcal pneumonia and meningitis. Every year, Cryptococcus neoformans endanger the lives of immunosuppressed hosts, resulting in 180,000 deaths per year. Nonetheless, healthy individuals can also be affected by this fungal infection. Cryptococcosis has a restricted and expensive therapeutic regimen with no topical approach to skin manifestations. This study sought to create a 3D printable biodegradable polymeric hydrogel carrying ketoconazole, a low‐cost antifungal drug with reported anticryptococcal activity. The developed hydrogel exhibited good 3D printability and rheological properties, including a pseudoplastic behavior. The FTIR spectra of cross‐linked hydrogels revealed interactions between alginate and Ca+2, referred to as the egg‐box model, indicated by the decrease in peaks at 1600 and 1410 cm−1. Furthermore, the hydrogel loaded with ketoconazole showed remarkable antifungal activity against C. neoformans strains indicated by inhibition zones, which cross‐linking did not seem to affect its antifungal performance. The developed material remained structurally stable for up to 12 days (288 h) in swelling studies, and preliminary cytotoxicity performed with V79 cells indicates potential for in vivo studies and topical application.
Beyond financials: Examining the impact of customer focus, internal processes, and learning & growth on the sustainable performance of commercial banks—Moderating role of management commitment
Authors: Ayele Nathenael Fentaw , Singh Manjit
Published: October 2024

This study examines the key factors influencing sustainable performance in commercial banks, focusing on the impact of non‐financial metrics—customer focus, internal processes, and learning and growth—within the Balanced Scorecard framework on the performance of commercial banks in Ethiopia. Additionally, it examines the moderating role of management commitment in this relationship, grounded in organizational learning theory, upper echelons theory, and the balanced scorecard model. The study adopts an explanatory research design, utilizing covariance‐based structural equation modeling and interaction‐term analysis. A multi‐stage sampling technique, followed by systematic random sampling, was employed, with Soper's formula used to determine a sample size of 480 from a total population of 4990. Mahalanobis distance was applied to identify and remove biased responses. The findings reveal that non‐financial metrics—customer focus, internal processes, and learning and growth—positively affect commercial banks' sustainable performance, and management commitment strengthens this effect. Furthermore, the results empirically validate the proposed hypotheses, emphasizing the value of incorporating non‐financial metrics into performance measurement and highlighting the essential role of management commitment in ensuring their success. This research fills a gap in the literature on sustainable performance measurement within the Ethiopian banking sector and provides actionable insights for managers and policymakers.
Community Fútbol Coaches Working Together to Prevent Violence and Promote Positive Youth Development in Colombia
Authors: De la Vega‐Taboada Eduardo , Guerra Ana Maria , Rieder Erica , Frazier Stacy L. , Cruz José Miguel , Jalali Mohammad S. , Stephens Dionne P.
Published: October 2024

In resource‐limited settings in Colombia, there is a lack of safe spaces for youth, with adolescent males being 10 times more susceptible to physical violence than females. Acknowledging the potential of community‐led sports‐based interventions, we examined how community fútbol (a.k.a. soccer or football) coaches in the Caribbean region of Colombia prevent youth violence exposure. By conducting in‐depth qualitative interviews with 13 community coaches, we explore how fútbol, recognised as the world's most popular sport, serves as a space and tool for violence prevention. Our mixed methods study employs qualitative interviews and social network analysis (SNA). The findings reveal that the community's vulnerability, including familial violence and drug use, has detrimental effects on children. Community coaches, positioned as trusted figures, strive to positively influence youth by instilling essential life skills. However, they face challenges such as resource scarcity, limited institutional support and financial difficulties. The coaches express the need to balance adolescents' socioemotional development and the competitive nature of tournaments (olympism). Moreover, a disconnection between community coaches and NGOs utilising Fútbol for Development stems from differing aims. We argue that collaboration between these two groups holds ample opportunities for mutual benefit and enhanced youth impact.
Oxidative Aromatization of Ethane
Authors: Damps Alexander , Roessner Frank
Published: October 2024

This study is focused on examining the incorporation of oxidative dehydrogenation into the aromatization of ethane, utilizing thermodynamic analysis and catalytic experiments. The catalysts were characterized by inverse temperature programmed reduction, X‐ray photoelectron spectroscopy (XPS) and X‐ray diffraction (XRD). The results indicated that a blend of the M1 catalyst, containing oxides of vanadium, niobium, and tellurium, with H‐ZSM‐5, serves as an effective catalyst system for the oxidative aromatization of ethane at T = 380 °C. The M1's role in the oxidative dehydrogenation of ethane contributes to de‐bottlenecking the essential step of the reaction. On the zeolitic catalyst aromatic compounds are formed from a surface hydrocarbon pool. In parallel, the oxidation of these intermediates was observed. Also, the formation of paraffins through H‐transfer was evident from the catalytic results. Although the zeolite underwent significant deactivation due to coking, the M1 catalyst demonstrated highly stable activity. Interestingly, the system did not show any synergistic effects. Based on the structure‐activity relation of the catalytic system a reaction mechanism is proposed.