bluuebunny/crossref_metadata_2025_split huggingface dataset:
Macromolecular Cargo Encapsulation via In Vitro Assembly of Two‐Component Protein Nanoparticles
Authors: Herpoldt Karla‐Luise , López Ciana L. , Sappington Isaac , Pham Minh N. , Srinivasan Selvi , Netland Jason , Montgomery Katherine S. , Roy Debashish , Prossnitz Alexander N. , Ellis Daniel , Wargacki Adam J. , Pepper Marion , Convertine Anthony J. , Stayton Patrick S. , King Neil P. 
Published: January 2024

AbstractSelf‐assembling protein nanoparticles are a promising class of materials for targeted drug delivery. Here, the use of a computationally designed, two‐component, icosahedral protein nanoparticle is reported to encapsulate multiple macromolecular cargoes via simple and controlled self‐assembly in vitro. Single‐stranded RNA molecules between 200 and 2500 nucleotides in length are encapsulated and protected from enzymatic degradation for up to a month with length‐dependent decay rates. Immunogenicity studies of nanoparticles packaging synthetic polymers carrying a small‐molecule TLR7/8 agonist show that co‐delivery of antigen and adjuvant results in a more than 20‐fold increase in humoral immune responses while minimizing systemic cytokine secretion associated with free adjuvant. Coupled with the precise control over nanoparticle structure offered by computational design, robust and versatile encapsulation via in vitro assembly opens the door to a new generation of cargo‐loaded protein nanoparticles that can combine the therapeutic effects of multiple drug classes.
3D Hydrogel Encapsulation Regulates Nephrogenesis in Kidney Organoids
Authors: Nerger Bryan A. , Sinha Sumit , Lee Nathan N. , Cheriyan Maria , Bertsch Pascal , Johnson Christopher P. , Mahadevan L. , Bonventre Joseph V. , Mooney David J. 
Published: January 2024

AbstractStem cell‐derived kidney organoids contain nephron segments that recapitulate morphological and functional aspects of the human kidney. However, directed differentiation protocols for kidney organoids are largely conducted using biochemical signals to control differentiation. Here, the hypothesis that mechanical signals regulate nephrogenesis is investigated in 3D culture by encapsulating kidney organoids within viscoelastic alginate hydrogels with varying rates of stress relaxation. Tubular nephron segments are significantly more convoluted in kidney organoids differentiated in encapsulating hydrogels when compared with those in suspension culture. Hydrogel viscoelasticity regulates the spatial distribution of nephron segments within the differentiating kidney organoids. Consistent with these observations, a particle‐based computational model predicts that the extent of deformation of the hydrogel–organoid interface regulates the morphology of nephron segments. Elevated extracellular calcium levels in the culture medium, which can be impacted by the hydrogels, decrease the glomerulus‐to‐tubule ratio of nephron segments. These findings reveal that hydrogel encapsulation regulates nephron patterning and morphology and suggest that the mechanical microenvironment is an important design variable for kidney regenerative medicine.
Anion‐Regulated Sulfur Conversion in High‐Content Carbon Layer Confined Sulfur Cathode Maximizes Voltage and Rate Capability of K–S Batteries
Authors: Jiang Zuobei , Li Na , Li Lingyi , Tan Feiming , Huang Junxi , Huang Shaoming 
Published: January 2024

AbstractPotassium–sulfur (K–S) batteries have attracted attention in large‐scale energy storage systems. Small‐molecule/covalent sulfur (SMCS) can help to avoid the shuttle effect of polysulfide ions via solid–solid sulfur conversion. However, the content of SMCS is relatively low (≤40%), and solid–solid reactions cause sluggish kinetics and low discharge potentials. Herein, SMCS is confined in turbo carbon layers with a content of ≈74.1 wt% via a C/S co‐deposition process. In the K–S battery assembled by using as‐fabricated SMCS@C as cathode and KFSI‐EC/DEC as an electrolyte, anion‐regulated two‐plateau solid‐state S conversion chemistry and a novel high discharge potential plateau at 2.5–2.0 V with a remarkable reversible capacity of 384 mAh g−1 at 3 A g−1 after 1000 cycles are found. The SMCS@C||K full cell showed energy and power density of 72.8 Wh kg−1 and 873.2 W kg−1, respectively, at 3 A g−1. Mechanism studies reveal that the enlarged carbon layer space enables the diffusion of K+‐FSI‐ ion pairs, and the coulombic attraction between them accelerates their diffusion in SMCS@C. In addition, FSI− regulates sulfur conversion in situ inside the carbon layers along a two‐plateau solid‐state reaction pathway, which lowers the free energy and weakens the S─S bond of intermediates, leading to faster and more efficient S conversion.
Dynamic Transition between Monomer and Excimer Phosphorescence in Organic Near‐Infrared Phosphorescent Crystals
Authors: Deng Zihao , Zhang Jianyu , Zhou Jiaming , Shen Wei , Zuo Yunfei , Wang Jin , Yang Shengyi , Liu Junkai , Chen Yuyang , Chen Chun‐Chao , Jia Guocheng , Alam Parvej , Lam Jacky W. Y. , Tang Ben Zhong 
Published: January 2024

AbstractAchieving efficient near‐infrared room‐temperature phosphorescence of purely organic phosphors remains scarce and challenging due to strong nonradiative decay. Additionally, the investigation of triplet excimer phosphorescence is rarely reported, despite the fact that excimer, a special emitter commonly formed in crystals with strong π–π interactions, can efficiently change the fluorescent properties of compounds. Herein, a series of dithienopyrrole derivatives with low triplet energy levels and stable triplet states, exhibiting persistent near‐infrared room‐temperature phosphorescence, is developed. Via the modification of halogen atoms, the crystals display tunable emissions of monomers from 645 to 702 nm, with a maximum lifetime of 3.68 ms under ambient conditions. Notably, excimer phosphorescence can be switched on at low temperatures, enabled by noncovalent interactions rigidifying the matrix and stabilizing triplet excimer. Unprecedentedly, the dynamic transition process is captured between the monomer and excimer phosphorescence with temperature variations, revealing that the unstable triplet excimers in crystals with a tendency to dissociate can result in the effective quench of room‐temperature phosphorescence. Excited state transitions across varying environments are elucidated, interpreting the structural dynamics of the triplet excimer and demonstrating strategies for devising novel near‐infrared phosphors.
Single‐Atom Alloys Materials for CO2 and CH4 Catalytic Conversion
Authors: He Chengxuan , Gong Yalin , Li Songting , Wu Jiaxin , Lu Zhaojun , Li Qixin , Wang Lingzhi , Wu Shiqun , Zhang Jinlong 
Published: January 2024

AbstractThe catalytic conversion of greenhouse gases CH4 and CO2 constitutes an effective approach for alleviating the greenhouse effect and generating valuable chemical products. However, the intricate molecular characteristics characterized by high symmetry and bond energies, coupled with the complexity of associated reactions, pose challenges for conventional catalysts to attain high activity, product selectivity, and enduring stability. Single‐atom alloys (SAAs) materials, distinguished by their tunable composition and unique electronic structures, confer versatile physicochemical properties and modulable functionalities. In recent years, SAAs materials demonstrate pronounced advantages and expansive prospects in catalytic conversion of CH4 and CO2. This review begins by introducing the challenges entailed in catalytic conversion of CH4 and CO2 and the advantages offered by SAAs. Subsequently, the intricacies of synthesis strategies employed for SAAs are presented and characterization techniques and methodologies are introduced. The subsequent section furnishes a meticulous and inclusive overview of research endeavors concerning SAAs in CO2 catalytic conversion, CH4 conversion, and synergy CH4 and CO2 conversion. The particular emphasis is directed toward scrutinizing the intricate mechanisms underlying the influence of SAAs on reaction activity and product selectivity. Finally, insights are presented on the development and future challenges of SAAs in CH4 and CO2 conversion reactions.
Precise Manipulation the Efficient Multi‐Exciton Emission with High Thermal Stability in Hybrid Manganese‐Antimony Chloride for Optical Thermometry, Anti‐Counterfeiting, and Information Encryption
Authors: Huang Tao , Wei Qilin , Li Tongzhou , Niu Quan , Li Weijian , Huang Guanhan , Zou Bingsuo 
Published: January 2024

AbstractRecently, zero‐dimensional (0D) metal halides with highly efficient tunable emission have shown broad prospects in the field of anti‐counterfeiting. However, the limited emission colors and low resolution, as well as the severe thermal quenching of self‐trapped excitons, have greatly constrained their applications. In this study, a high thermal stability compound by precisely manipulating the multi‐exciton emission within Sb‐doped hybrid manganese chloride is developed, which exhibits three emission colors (green, orange, and yellow). It is discovered that this compound exhibits significant color changes in the low‐temperature range. Optical temperature sensing, anti‐counterfeiting, and information encryption models based on this compound are successfully designed. This research proposes an effective strategy for designing novel eco‐friendly and efficient anti‐counterfeiting and temperature sensing materials, paving the way for optical temperature sensing and multi‐key encryption‐decryption applications.
Electronic and Steric Effects in a Gold(I)‐Catalyzed Intramolecular C(sp3)−H Bond Activation Reaction of 1‐Bromoalkynes
Authors: Miguélez Rubén , Arto Omar , Semleit Nina , Haberhauer Gebhard , Barrio Pablo 
Published: January 2024

AbstractThe functional group compatibility of our recently disclosed gold(I)‐catalyzed cycloisomerization of 1‐bromoalkynes is studied in detail. Two main features are addressed, the minimum distances at which polar functional groups are tolerated and the influence of both electronic and steric effects on the performance of aryl ether derivatives. Moreover, robustness assessment experiments have been carried out shedding light on the factors dictating functional group tolerance. In addition, the reaction has been applied to the synthesis of a key intermediate in the total synthesis of a natural product and a heterobifunctional molecule. DFT calculations have shed light on the mechanistic features behind the observed reactivity trends. On one hand, the destabilization of the TS by the proximity of the polar group may hamper the reactivity for proximal functional groups. On the other hand, some polar functional groups are not tolerated regardless of their position due to the preferential coordination of gold to the oxygen atom over the alkyne, resulting presumably in competitive catalyst deactivation pathways.
Chaotropic Nanoelectrocatalysis: Chemically Disrupting Water Intermolecular Network at the Point‐of‐Catalysis to Boost Green Hydrogen Electrosynthesis
Authors: Ng Li Shiuan , Chah Eu Li Chloe , Ngieng Min Hui , Boong Siew Kheng , Chong Carice , Raja Mogan Tharishinny , Lee Jinn‐Kye , Li Haitao , Lee Chi‐Lik Ken , Lee Hiang Kwee 
Published: January 2024

AbstractEfficient green hydrogen production through electrocatalytic water splitting serves as a powerful catalyst for realizing a carbon‐free hydrogen economy. However, current electrocatalytic designs face challenges such as poor hydrogen evolution reaction (HER) performance (Tafel slope, 100–140 mV dec−1) because water molecules are thermodynamically trapped within their extensive hydrogen bonding network. Herein, we drive efficient HER by manipulating the local water microenvironment near the electrocatalyst. This is achieved by functionalizing the nanoelectrocatalyst's surface with a monolayer of chaotropic molecules to chemically weaken water‐water interactions directly at the point‐of‐catalysis. Notably, our chaotropic design demonstrates a superior Tafel slope (77 mV dec−1) and the lowest overpotential (0.3 V at 10 mA cm−2ECSA), surpassing its kosmotropic counterparts (which reinforces the water molecular network) and previously reported electrocatalytic designs by up to ≈2‐fold and ≈3‐fold, respectively. Comprehensive mechanistic investigations highlight the critical role of chaotropic surface chemistry in disrupting the water intermolecular network, thereby releasing free/weakly bound water molecules that strongly interact with the electrocatalyst to boost HER. Our study provides a unique molecular approach that can be readily integrated with emerging electrocatalytic materials to rapidly advance the electrosynthesis of green hydrogen, holding immense promise for sustainable chemical and energy applications.
Regioselective Dearomative Amidoximation of Nonactivated Arenes Enabled by Photohomolytic Cleavage of N‐nitrosamides
Authors: Yuan Pan‐Feng , Huang Xie‐Tian , Long Linhong , Huang Tao , Sun Chun‐Lin , Yu Wei , Wu Li‐Zhu , Chen Hui , Liu Qiang 
Published: January 2024

AbstractDearomative spirocyclization reactions represent a promising means to convert arenes into three‐dimensional architectures; however, controlling the regioselectivity of radical dearomatization with nonactivated arenes to afford the spirocyclizative 1,2‐difunctionalization other than its kinetically preferred 1,4‐difunctionalization is exceptionally challenging. Here we disclose a novel strategy for dearomative 1,2‐ or 1,4‐amidoximation of (hetero)arenes enabled by direct visible‐light‐induced homolysis of N−NO bonds of nitrosamides, giving rise to various highly regioselective amidoximated spirocycles that previously have been inaccessible or required elaborate synthetic efforts. The mechanism and origins of the observed regioselectivities were investigated by control experiments and density functional theory calculations.
Pivotal Role of Geometry Regulation on O−O Bond Formation Mechanism of Bimetallic Water Oxidation Catalysts
Authors: Chen Qi‐Fa , Xian Ke‐Lin , Zhang Hong‐Tao , Su Xiao‐Jun , Liao Rong‐Zhen , Zhang Ming‐Tian 
Published: January 2024

AbstractIn this study, we highlight the impact of catalyst geometry on the formation of O−O bonds in Cu2 and Fe2 catalysts. A series of Cu2 complexes with diverse linkers are designed as electrocatalysts for water oxidation. Interestingly, the catalytic performance of these Cu2 complexes is enhanced as their molecular skeletons become more rigid, which contrasts with the behavior observed in our previous investigation with Fe2 analogs. Moreover, mechanistic studies reveal that the reactivity of the bridging O atom results in distinct pathways for O−O bond formation in Cu2 and Fe2 catalysts. In Cu2 systems, the coupling takes place between a terminal CuIII−OH and a bridging μ−O⋅ radical. Whereas in Fe2 systems, it involves the coupling of two terminal Fe–oxo entities. Furthermore, an in‐depth structure–activity analysis uncovers the spatial geometric prerequisites for the coupling of the terminal OH with the bridging μ−O⋅ radical, ultimately leading to the O−O bond formation. Overall, this study emphasizes the critical role of precisely adjusting the spatial geometry of catalysts to align with the O−O bonding pathway.
Polymeric Metal Halides with Bright Luminescence and Versatile Processability
Authors: Li Shun‐Shun , Cheng Pengfei , Liu Huaxin , Li Juntao , Wang Sijia , Xiao Chunlei , Liu Jianyong , Chen Junsheng , Wu Kaifeng 
Published: January 2024

AbstractMost of current metal halide materials, including all inorganic and organic–inorganic hybrids, are crystalline materials with poor workability and plasticity that limit their application scope. Here, we develop a novel class of materials termed polymeric metal halides (PMHs) through introducing polycations into antimony‐based metal halide materials as A‐site cations. A series of PMHs with orange‐yellow broadband emission and large Stokes shift originating from inorganic self‐trapped excitons are successfully prepared, which meanwhile exhibit the excellent processability and formability of polymers. The versatility of these PMHs is manifested as the broad choices of polycations, the ready extension to manganese‐ and copper‐based halides, and the tolerance to molar ratios between polycations and metal halides in the formation of PMHs. The merger of polymer chemistry and inorganic chemistry thus provides a novel generic platform for the development of metal halide functional materials.
Transboundary fine dust pollution in China and Korea: How has international politics impeded environmental negotiations?
Authors: Zhang Muhui 
Published: January 2024

AbstractTransboundary fine dust has been a leading cause of dispute between China and Korea since the mid‐2010s. This study observes that transboundary fine dust is not purely an environmental issue, but rather mixed with political and diplomatic challenges. Despite the emerging bilateral and multilateral efforts to tackle this issue, this research sheds light on how political and diplomatic factors have undermined the outcomes of environmental negotiations between China and Korea. We highlight three dimensions of policy‐based studies: scientific joint research on source‐receptor relationships, interstate environmental negotiations, and multilateral environmental institutions in Northeast Asia. This study argues that transboundary fine dust cooperation has been extensively entangled with national political interests and proceeded via diplomatic channels, leading to the current absence of binding agreements and policy commitments. Therefore, a steady process of de‐linking environmental cooperation and diplomatic fluctuations would be the best direction to proceed in a long‐term perspective.
A Review of Degradation Mechanisms and Recent Achievements for Na‐Ion Layered Transition Metal Oxides
Authors: Feng Jiameng , Fang De , Li Jie , Li Jianling 
Published: January 2024

AbstractDue to the low price and high specific capacity, sodium ion batteries (SIBs) have become a crucial candidate for the future large‐scale energy storage power station, providing strong support for energy transition. Layered transition metal oxides (LTMOs), as one of the most promising cathode materials for SIBs, are usually accompanied by the sodiation/de‐sodiation during charging/discharging, which leads to the slippage and deformation of the layered structure, and consequently causes to the degradation of electrochemical performance. The degradation mechanisms of LTMOs attributed to the structural change are important references for improving the electrochemical performance of cathode materials. Here, this paper presents the main degradation mechanisms such as irreversible anion redox reaction, Na+/vacancy ordering transition and poor air stability as well as the corresponding modification means. It also summarizes the challenges faced by sodium‐ion LTMOs cathode materials, and gives an outlook on the key issues that need to be solved for future development.
A red fluorescent carbon dots with good water solubility for rapid detection of Al3+ in actual samples
Authors: Zhao Jingyuan , Yao Jie , Wang Yingqi , Wang Ning , Wang Jianhua 
Published: January 2024

AbstractWe developed a facile strategy for the fabrication of red fluorescent carbon nanodots (R‐CDs) and demonstrated their applications for Al3+ sensing. Red‐emission carbon dots (CDs) were synthesized using a simple hydrothermal treatment with citric acid and urea as precursors, manifesting intriguing red‐emission behaviour at 610 nm. With increasing Al3+ concentration, the fluorescence band at 610 nm decreased gradually. Monitoring the intrinsic fluorescence variation (I610nm), as‐prepared CDs were developed as an effective platform for fluorescent Al3+ sensing, with a linear range of 0.5–60.0 μM and a detection limit of 3.0 nM. More importantly, R‐CDs have been applied successfully to the analysis of Al3+ in actual samples with satisfactory recoveries in the range 97.12–102.05%, which indicated that obtained CDs could be implemented as an effective tool for the identification and detection of Al3+ in actual samples.
Recombinant protein expression in proteome‐reduced cells under aerobic and oxygen‐limited regimes
Authors: Lara Alvaro R. , Utrilla Jose , Martínez Luz María , Krausch Niels , Kaspersetz Lucas , Hidalgo David , Cruz‐Bournazou Nicolas , Neubauer Peter , Sigala Juan‐Carlos , Gosset Guillermo , Büchs Jochen 
Published: January 2024

AbstractIndustrial cultures are hindered by the physiological complexity of the host and the limited mass transfer capacity of conventional bioreactors. In this study, a minimal cell approach was combined with genetic devices to overcome such issues. A flavin mononucleotide‐based fluorescent protein (FbFP) was expressed in a proteome‐reduced Escherichia coli (PR). When FbFP was expressed from a constitutive protein generator (CPG), the PR strain produced 47% and 35% more FbFP than its wild type (WT), in aerobic or oxygen‐limited regimes, respectively. Metabolic and expression models predicted more efficient biomass formation at higher fluxes to FbFP, in agreement with these results. A microaerobic protein generator (MPG) and a microaerobic transcriptional cascade (MTC) were designed to induce FbFP expression upon oxygen depletion. The FbFP fluorescence using the MTC in the PR strain was 9% higher than that of the WT bearing the CPG under oxygen limitation. To further improve the PR strain, the pyruvate dehydrogenase complex regulator gene was deleted, and the Vitreoscilla hemoglobin was expressed. Compared to oxygen‐limited cultures of the WT, the engineered strains increased the FbFP expression more than 50% using the MTC. Therefore, the designed expression systems can be a valuable alternative for industrial cultivations.
Index of Microcirculatory Resistance to predict microvascular obstruction in STEMI: A systematic review and meta‐analysis
Authors: Jeyaprakash Prajith , Mikhail Philopatir , Ford Thomas J. , Pathan Faraz , Berry Colin , Negishi Kazuaki 
Published: January 2024

AbstractBackgroundMicrovascular obstruction (MVO) is an independent predictor of adverse cardiac events after ST‐elevation myocardial infarction (STEMI). The Index of Microcirculatory Resistance (IMR) may be a useful marker of MVO, which could simplify the care pathway without the need for Cardiac Magnetic Resonance (CMR). We assessed whether the IMR can predict MVO in STEMI patients.Methods and ResultsWe conducted a systematic review and meta‐analysis, including articles where invasive IMR was performed post primary percutaneous coronary intervention (PCI) in addition to MVO assessment with cardiac MRI. We searched PubMed, Scopus, Embase, and Cochrane databases from inception until January 2023. Baseline characteristics, coronary physiology and cardiac MRI data were extracted by two independent reviewers. The random‐effects model was used to pool the data. Among 15 articles identified, nine articles (n = 728, mean age 61, 81% male) contained IMR data stratified by MVO. Patients with MVO had a mean IMR of 41.2 [95% CI 32.4−50.4], compared to 25.3 [18.3−32.2] for those without. The difference in IMR between those with and without MVO was 15.1 [9.7−20.6]. Meta‐regression analyses demonstrated a linear relationship between IMR and TIMI grade (β = 0.69 [0.13−1.26]), as well as infarct size (β = 1.18 [0.24−2.11]) or ejection fraction at 6 months (β = −0.18 [−0.35 to −0.01]).ConclusionIn STEMI, patients with MVO had 15‐unit higher IMR than those without. IMR also predicts key prognostic endpoints such as infarct size, MVO, and long‐term systolic function.