bluuebunny/crossref_metadata_2025_split huggingface dataset:
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

AbstractThe 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

AbstractPristine 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

AbstractThe 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

AbstractBiodegradable 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

AbstractSmart 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

AbstractSince 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

AbstractAn 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

AbstractDeuterated 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

AbstractPolyethyleneimine (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

AbstractDynamic 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

AbstractAlbuminuria 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.
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

AbstractProtein 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

AbstractThe 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

AbstractQuantum 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

AbstractMolecularly‐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.