bluuebunny/crossref_metadata_2025_split huggingface dataset:
Enhancing the Photocatalytic Activity of Zirconium‐Based Metal–Organic Frameworks Through the Formation of Mixed‐Valence Centers
Authors: Wei Zihao , Song Shaojia , Gu Hongfei , Li Yaqiong , Sun Qi , Ding Ning , Tang Hao , Zheng Lirong , Liu Shuhu , Li Zhenxing , Chen Wenxing , Li Shenghua , Pang Siping 
Published: August 2023

AbstractDespite the desirability of metal–organic frameworks (MOFs) as heterogeneous photocatalysts, current strategies available to enhance the performance of MOF photocatalysts are complicated and expensive. Herein, a simple strategy is presented for improving the activity of MOF photocatalysts by regulating the atomic interface structure of the metal active sites on the MOF. In this study, MOF (PCN‐222) is hybridized with cellulose acetate (CA@PCN‐222) through an optimized atomic interface strategy, which lowers the average valence state of Zr ions. The electronic metal‐support interaction mechanism of CA@PCN‐222 is revealed by evaluating the photocatalytic CO2 reduction reaction (CO2RR). The experimental results suggested that the electron migration efficiency at the atomic interface of the MOFs strongly coupled with cellulose is significantly improved. In particular, the CO2RR to formate activity of CA@PCN‐222 photocatalyst greatly increased from 778.2 to 2816.0 µmol g−1 compared with pristine PCN‐222 without cellulose acetate. The findings suggest that the strongly coupled metal–ligand moiety at the atomic interface of MOFs may play a synergistic role in heterogeneous catalysts.
Untethered Magnetic Soft Robot with Ultra‐Flexible Wirelessly Rechargeable Micro‐Supercapacitor as an Onboard Power Source
Authors: Nardekar Swapnil Shital , Kim Sang‐Jae 
Published: August 2023

AbstractSoft robotics has developed rapidly in recent years as an emergent research topic, offering new avenues for various industrial and biomedical settings. Despite these advancements, its applicability is limited to locomotion and actuation due to the lack of an adequate charge storage system that can support the robot's sensory system in challenging conditions. Herein, an ultra‐flexible, lightweight (≈50 milligrams), and wirelessly rechargeable micro‐supercapacitor as an onboard power source for miniaturized soft robots, capable of powering a range of sensory is proposed. The simple and scalable direct laser combustion technique is utilized to fabricate the robust graphene‐like carbon micro‐supercapacitor (GLC‐MSC) electrode. The GLC‐MSC demonstrates superior areal capacitance (8.76 mF cm−2), and maintains its original capacitance even under extreme actuation frequency (1–30 Hz). As proof of conceptthe authors fabricate a fully integrated magnetic‐soft robot that shows outstanding locomotion aptitude and charged wirelessly (up to 2.4 V within 25s), making it an ideal onboard power source for soft robotics.
Intra‐Operative Definition of Glioma Infiltrative Margins by Visualizing Immunosuppressive Tumor‐Associated Macrophages
Authors: Cao Chong , Yin Hang , Yang Biao , Yue Qi , Wu Guoqing , Gu Meng , Zhang Yuwen , Fan Yang , Dong Xiaoyan , Wang Ting , Wang Cong , Zhu Xiao , Mao Ying , Zhang Xiao‐Yong , Lei Zuhai , Li Cong 
Published: August 2023

AbstractAccurate delineation of glioma infiltrative margins remains a challenge due to the low density of cancer cells in these regions. Here, a hierarchical imaging strategy to define glioma margins by locating the immunosuppressive tumor‐associated macrophages (TAMs) is proposed. A pH ratiometric fluorescent probe CP2‐M that targets immunosuppressive TAMs by binding to mannose receptor (CD206) is developed, and it subsequently senses the acidic phagosomal lumen, resulting in a remarkable fluorescence enhancement. With assistance of CP2‐M, glioma xenografts in mouse models with a tumor‐to‐background ratio exceeding 3.0 for up to 6 h are successfully visualized. Furthermore, by intra‐operatively mapping the pH distribution of exposed tissue after craniotomy, the glioma allograft in rat models is precisely excised. The overall survival of rat models significantly surpasses that achieved using clinically employed fluorescent probes. This work presents a novel strategy for locating glioma margins, thereby improving surgical outcomes for tumors with infiltrative characteristics.
Thermal Stability of Sulfide Solid Electrolyte with Lithium Metal
Authors: Wu Yujing , Xu Jing , Lu Pushun , Lu Jiaze , Gan Luyu , Wang Shuo , Xiao Ruijuan , Li Hong , Chen Liquan , Wu Fan 
Published: August 2023

AbstractAll solid–state battery (ASSB) is widely recognized as one of the most promising high‐energy‐density systems/technologies. However, thermal safety issues induced by highly reactive materials still exist for solid electrolytes (SEs). Insights on thermal behaviors at elevated temperatures and the underlying mechanism for thermal stability of SE‐based systems are still missing. Herein, thermal stability performance of typical sulfide SEs is systematically investigated with metal Li, whose order of interfacial thermal stability is concluded to be Li6PS5Cl > Li3PS4 > Li9.54Si1.74P1.44S11.7Cl0.3 > Li4SnS4 > Li7P3S11 after a comprehensive evaluation. Interestingly, Li4SnS4, which achieves good air stability, has poor thermal stability with Li metal. This is possibly caused by Li─Sn alloy products generated during thermal decomposition, and their great thermodynamic driving force towards SE for accelerated thermal runaway. Moreover, electrolytes with poor material‐level thermal stability (e.g., Li7P3S11) may form a dense passivation layer by self‐decomposition with Li metal to retard thermal runaway. Conclusively, the material structure affects the thermodynamic stability of the system, but the reaction products (interphase) affects the kinetic process of the thermal reaction within a certain temperature range. Therefore, thermal stability with both metallic lithium and decomposition products is a necessary condition for interfacial thermal stability of sulfide SEs.
Self‐Healing of Proton‐Irradiated Organic Photodiodes and Photovoltaics
Authors: Parkhomenko Hryhorii P. , Mostovyi Andriy I. , Akhtanova Gulnur , Solovan Mykhailo M. , Kaikanov Marat , Schopp Nora , Brus Viktor V. 
Published: August 2023

AbstractIn this study, a comprehensive quantitative analysis of the photodiode (PD) is conducted and photovoltaic (PV) characteristics of organic non‐fullerene PCE10:ITIC‐4F devices before and after exposure to a 150 ns pulse of 170 keV proton irradiation with the fluence of 2·1012 p cm−2 that is equivalent to ≈6 years of operation at a low Earth orbit. While an expected initial performance reduction happened in the photodiode and photovoltaic operation modes, a hitherto unknown self‐healing effect in the organic devices is observed several days after the proton irradiation. The organic bulk‐heterojunction (BHJ) material properties and the multi‐mechanisms recombination processes before and after irradiation and during self‐healing are investigated. This analysis provides a quantitative understanding of the changes occurring in the device physics and points toward the relevant aspects of the self‐healing mechanism related to the dynamics of proton‐induced traps in the bulk of the organic active layer. Ultimately, the synergy of record lightweight features and newly discovered self‐healing of proton‐induced damage in organic PDs and solar cells highlights their great potential for applications in rapidly emerging space technology.
Review of Emerging Atomically Precise Composite Site‐Based Electrocatalysts
Authors: Yang Xinyi , Song Wanqing , Zhang Tao , Huang Zechuan , Zhang Jinfeng , Ding Jia , Hu Wenbin 
Published: August 2023

AbstractAtomically precise composite site‐based catalysts with new electrocatalytic synergistic mechanisms and enhanced electrocatalytic activities have emerged as a frontier in the electrocatalysis community. This topical review focuses on the recent research advances of atomically precise metal composite sites‐based electrocatalysts. This work first demonstrates an overview of the configurations of atomically precise composite sites, including a discussion of the advanced methods employed for understanding the composite sites. The review then provides a comprehensive organization of the previously reported methodologies of synthesizing electrocatalysts with atomically precise composite sites. Representative case studies are provided, starting from the simple one‐step pyrolysis strategy to the species‐by‐species multi‐step pyrolysis strategy. Based on the preceding discussions of the catalyst materials, the review further discusses the unique electrocatalysis mechanisms raised by the composite sites, that are different from the routine single species sites. The electrocatalytic systems mainly involve the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, nitrogen reduction reaction, and carbon dioxide reduction reaction. The themes of this section include the true active center determination for composite sites and various types of electrocatalytic synergy mechanisms. Finally, critical unanswered questions and remaining challenges, as well as promising underexplored research directions are identified.
The prevalence of frailty and its relationship with sociodemographic factors, regional healthcare disparities, and healthcare utilization in the aging population across India
Authors: Singhal Sunny , Singh Sumitabh , Dewangan Gevesh Chand , Dey Sharmistha , Banerjee Joyita , Lee Jinkook , Upadhyaya Ashish Datt , Hu Peifeng , Dey Aparajit Ballav 
Published: August 2023

AbstractObjectiveTo estimate frailty prevalence and its relationship with the socio‐economic and regional factors and health care outcomes.MethodsIn this study, participants from the harmonized Diagnostic Assessment of Dementia for the Longitudinal Aging Study in India (LASI‐DAD) were included. The frailty index (FI) was calculated using a 32‐variable deficit model, with a value of ≥ 25% considered as frail. Data on demographic (including caste and religion) and socioeconomic profiles and health care utilization were obtained. The state‐wise health index maintained by the government based on various health‐related parameters was used to group the participants' residential states into high‐, intermediate‐, and low‐performing states. Multivariable and zero‐inflated negative binomial regression was used to assess the relationship of frailty index with sociodemographic characteristics, health index, and health care expenditure or hospitalization.ResultsAmong the 3953 eligible participants, the prevalence of frailty was 42.34% (men = 34.99% and women = 49.35%). Compared to high‐performing states, intermediate‐ and low‐performing states had a higher proportion of frail individuals (49.7% vs. 46.8% vs. 34.5%, P < 0.001). In the adjusted analysis, frailty was positively associated with age, female sex, rural locality, lower education level, and caste (scheduled caste and other backward classes). After adjusting for the socio‐economic profile, FI was inversely associated with the composite health index of a state (P < 0.001). FI was also significantly correlated with total 1‐year health care expenditure and hospitalization (P < 0.001 and 0.020, respectively).ConclusionThere is a high prevalence of frailty among older Indian adults that is associated with sociodemographic factors and regional health care performance. Furthermore, frailty is associated with increased health care utilization and expenditure.
Self‐assembly multifunctional DNA tetrahedron for efficient elimination of antibiotic‐resistant bacteria
Authors: Wu Tiantian , Fu Yu , Guo Shuang , Shi Yanqiang , Zhang Yuxin , Fan Zhijin , Yang Bin , Ding Baoquan , Liao Yuhui 
Published: August 2023

AbstractAntibiotic resistance is a major challenge in the clinical treatment of bacterial infectious diseases. Herein, we constructed a multifunctional DNA nanoplatform as a versatile carrier for bacteria‐specific delivery of clinical antibiotic ciprofloxacin (CIP) and classic nanoantibiotic silver nanoparticles (AgNP). In our rational design, CIP was efficiently loaded in the self‐assembly double‐bundle DNA tetrahedron through intercalation with DNA duplex, and single‐strand DNA‐modified AgNP was embedded in the cavity of the DNA tetrahedron through hybridization. With the site‐specific assembly of targeting aptamer in the well‐defined DNA tetrahedron, the bacteria‐specific dual‐antibiotic delivery system exhibited excellent combined bactericidal properties. With enhanced antibiotic accumulation through breaking the out membrane of bacteria, the antibiotic delivery system effectively inhibited biofilm formation and promoted the healing of infected wounds in vivo. This DNA‐based antibiotic delivery system provides a promising strategy for the treatment of antibiotic‐resistant infections.
Experimental and computational design tools for industrial drying processes: Challenges in process‐limit prediction
Authors: Parrish Chance , Bell Nelson , Larsen Marvin E. , Tjiptowidjojo Kristianto , Schunk P. Randall 
Published: August 2023

AbstractThe coating and drying of inks and slurries are important steps to manufacture a plethora of products. Drying processes, particularly, comprise energy‐intensive steps that affect product cost and quality. Prior work has highlighted failures of various multicomponent diffusivity models to conserve mass in dryer modeling and challenges in predicting process limits given variability in published values of key thermodynamic parameters. Herein, we develop a computational model and benchtop drying experiments to investigate these concerns for drying polymer‐laden coatings. Model predictions of process limits in a single‐zone drying oven demonstrate that published variability in Flory–Huggins parameter yields large variations in predicted operating temperatures above which blistering occurs. This indicates that caution should be exercised when choosing approaches to obtain or predict the Flory–Huggins parameter, and that both benchtop drying experiments and a set of additional experiments, such as sorption experiments, are needed to fully characterize and optimize a given drying process.
Cardiovascular health, infection burden, and incident dementia in the UK Biobank
Authors: Beydoun Hind A. , Beydoun May A. , Meirelles Osorio , Erickson Lance D. , Gamaldo Alyssa A. , Weiss Jordan , Launer Lenore J. , Evans Michele K. , Zonderman Alan B. 
Published: August 2023

AbstractINTRODUCTIONAmong older adults, total and hospitalized infection may be associated with incidence of all‐cause and Alzheimer's disease (AD) dementias, with variation by cardiovascular health (CVH).METHODSWe used Cox proportional hazards (PH) models to examine the relationships between International Classification of Diseases‐10th revision (ICD‐10)‐specific viral and bacterial infectious agents and incident all‐cause and AD dementia among 355,046 UK Biobank participants ≥50 years at baseline. Life's Essential 8 (LE8) index reflected CVH.RESULTSIn both sexes, total infection burden (yes vs. no) was associated with all‐cause dementia, with significant interactions by LE8 tertiles, whereby this relationship was significant only in the lowest LE8 tertile. Hospital‐treated infection burden (yes vs no) was significantly related to all‐cause and AD dementia, with no significant interaction with LE8 tertile. Age group patterns were detected.DISCUSSIONAD and all‐cause dementia were related to hospital‐treated infections, while CVH modified the relationship of total infection burden with all‐cause dementia.Highlights
Secondary analysis on >355,000 UK Biobank participants ≥50 years at baseline.
Alzheimer's disease and all‐cause dementia are both related to hospital‐treated infection.
Cardiovascular health modifies association of infection burden with all‐cause dementia.
Severity of GNAO1‐Related Disorder Correlates with Changes in G‐Protein Function
Authors: Domínguez‐Carral Jana , Ludlam William Grant , Junyent Segarra Mar , Fornaguera Marti Montserrat , Balsells Sol , Muchart Jordi , Čokolić Petrović Dunja , Espinoza Iván , Ortigoza‐Escobar Juan Dario , Martemyanov Kirill A. ,   GNAO1‐Study Group
Published: August 2023

ObjectiveGNAO1‐related disorders (OMIM #615473 and #617493), caused by variants in the GNAO1 gene, are characterized by developmental delay or intellectual disability, hypotonia, movement disorders, and epilepsy. Neither a genotype–phenotype correlation nor a clear severity score have been established for this disorder. The objective of this prospective and retrospective observational study was to develop a severity score for GNAO1‐related disorders, and to delineate the correlation between the underlying molecular mechanisms and clinical severity.MethodsA total of 16 individuals with GNAO1‐related disorders harboring 12 distinct missense variants, including four novel variants (p.K46R, p.T48I, p.R209P, and p.L235P), were examined with repeated clinical assessments, video‐electroencephalogram monitoring, and brain magnetic resonance imaging. The molecular pathology of each variant was delineated using a molecular deconvoluting platform.ResultsThe patients displayed a wide variability in the severity of their symptoms. This heterogeneity was well represented in the GNAO1‐related disorders severity score, with a broad range of results. Patients with the same variant had comparable severity scores, indicating that differences in disease profiles are not due to interpatient variability, but rather, to unique disease mechanisms. Moreover, we found a significant correlation between clinical severity scores and molecular mechanisms.InterpretationThe clinical score proposed here provides further insight into the correlation between pathophysiology and phenotypic severity in GNAO1‐related disorders. We found that each variant has a unique profile of clinical phenotypes and pathological molecular mechanisms. These findings will contribute to better understanding GNAO1‐related disorders. Additionally, the severity score will facilitate standardization of patients categorization and assessment of response to therapies in development. ANN NEUROL 2023;94:987–1004
Discovering Dynamic Plant Enzyme Complexes in Yeast for Kratom Alkaloid Pathway Identification**
Authors: Wu Yinan , Liu Chang , Koganitsky Anna , Gong Franklin L. , Li Sijin 
Published: August 2023

AbstractDiscovering natural product biosynthetic pathways of medicinal plants is challenging and laborious. Capturing the coregulation patterns of pathway enzymes, particularly transcriptomic regulation, has proven an effective method to accelerate pathway identification. In this study, we developed a yeast‐based screening method to capture the protein‐protein interactions (PPI) between plant enzymes, which is another useful pattern to complement the prevalent approach. Combining this method with plant multiomics analysis, we discovered four enzyme complexes and their organized pathways from kratom, an alkaloid‐producing plant. The four pathway branches involved six enzymes, including a strictosidine synthase, a strictosidine β‐D‐glucosidase (MsSGD), and four medium‐chain dehydrogenase/reductases (MsMDRs). PPI screening selected six MsMDRs interacting with MsSGD from 20 candidates predicted by multiomics analysis. Four of the six MsMDRs were then characterized as functional, indicating the high selectivity of the PPI screening method. This study highlights the opportunity of leveraging post‐translational regulation features to discover novel plant natural product biosynthetic pathways.
Die Rolle von unreaktiven Polyanionen in aktiven, chemisch regulierten komplexen Koazervaten
Authors: Späth Fabian , Maier Anton S. , Stasi Michele , Bergmann Alexander M. , Halama Kerstin , Wenisch Monika , Rieger Bernhard , Boekhoven Job 
Published: August 2023

AbstractKomplexe Koazervation beschreibt die Flüssig‐Flüssig‐Phasentrennung entgegengesetzt geladener Polymere. Aktive Koazervate sind Tröpfchen, in denen die Affinität eines der Elektrolyte durch chemische Reaktionen gesteuert wird. Diese Tröpfchen sind besonders interessant, weil ihre Eigenschaften durch die Reaktionskinetik streng reguliert werden. Sie dienen beispielsweise als Modell für membranlose Organellen, die häufig auch durch biochemische Transformationen, wie z. B. posttranslationale Modifikationen, gesteuert werden. Sie sind auch ein gutes Modell für Protozellen oder könnten zur Synthese von künstlichem Leben verwendet werden – sie entstehen spontan als Reaktion auf Reagenzien, konkurrieren und zerfallen, sobald alle Nährstoffe verbraucht sind. Allerdings ist die Rolle der unreaktiven Bausteine, z. B. der Polymere, bisher kaum verstanden. Mit unserer Arbeit zeigen wir die wichtige Rolle des unreaktiven Polyanions unserer chemisch betriebenen Koazervattropfen. Wir zeigen, dass das Polyanion den Lebenszyklus der resultierenden Tröpfchen drastisch beeinflusst, ohne den chemischen Reaktionszyklus selbst zu beeinflussen – entweder sind sie sehr dynamisch oder lösen sich nur verzögert auf. Darüber hinaus leiten wir den Mechanismus dahinter ab und zeigen, wie Additive und rationales Polymerdesign dazu beitragen können, die gewünschten Lebenszyklen von Koazervatemulsionen zu erzeugen.
Photoinduzierte Metallonitrenbildung durch N2 Abspaltung aus Azid‐Diradikal‐Liganden
Authors: Domenianni Luis I. , Bauer Markus , Schmidt‐Räntsch Till , Lindner Jörg , Schneider Sven , Vöhringer Peter 
Published: August 2023

AbstractÜbergangsmetallnitride/nitrene sind vielversprechende Reagenzien für katalytischen Stickstoffatomtransfer, die in situ durch optisch induzierte N2‐Eliminierung aus Azidkomplexen zugänglich sind. Um ihr synthetisches Potenzial für die Katalyse voll ausschöpfen zu können, ist ein grundlegendes Verständnis der primären photoinduzierten Prozesse und der stereoelektronischen Faktoren, welche die N2‐Dissoziation kontrollieren, unerlässlich. Mit Hilfe von Femtosekunden‐Infrarotspektroskopie klären wir hier die primären molekularen Mechanismen auf, die für die Bildung eines einzigartigen Platin(II)nitrens mit Triplett‐Grundzustand aus einem geschlossenschaligen Platin(II)azidkomplex verantwortlich sind. Die spektroskopischen Daten in Kombination mit quantenchemischen Rechnungen ergeben einen konsistenten Mechanismus: Produktbildung erfordert die anfängliche Besetzung eines angeregten Singulett‐Zustands mit anionischen Azid‐Diradikal‐Liganden, der an ein low‐spin d8‐konfiguriertes PtII‐Ion gebunden ist. Anschließende Interkombination erzeugt das an Platin gebundene Triplett‐Aziddiradikal, welches sich durch N2‐Verlust in einer nahezu barrierelosen, adiabatischen Dissoziation nahtlos in das Triplett‐Nitren umwandelt. Unsere Daten unterstreichen die Bedeutung des produktiven, N2‐freisetzenden Zustands mit Azid ππ* Charakter als Konstruktionsprinzip für den Zugang zu effizienten Stickstoffatomtransfer‐Katalysatoren.