bluuebunny/crossref_metadata_2025_split huggingface dataset:
Synergistic Pd‐Au Catalyst for Selective Electrosynthesis of Dimethyl Carbonate in Conjunction with High‐Rate Redox System
Authors: Fujinuma Naohiro , Page Natalie , Boddy Anna G , Rivkind Joshua , Tomlinson Lindsey , Hoy Erik P , Lofland Samuel E 
Published: September 2024

AbstractThis study reports ambient electrosynthesis of dimethyl carbonate with a palladium–gold catalyst. Material screening identifies a region of intermediate‐catalyst binding energy that facilitates interfacial electron and proton transfers for selective carbonylation, achieving a distinct maximum of 92% faradaic efficiency to dimethyl carbonate. Structural and electrochemical analyses suggest that the alloying of palladium and gold effectively modulates the CO* binding energy to the catalytic surface, in accord with subsequent computational studies. With an extended heterogeneous–homogeneous catalytic environment with a halide redox mediator, a remarkable partial current density of 52 mA cm−2 is observed for dimethyl carbonate for 100 h of continuous operation.
Modulating the Li‐Ion Transport Pathway of Succinonitrile‐Based Plastic Crystalline Electrolytes for Solid‐State Lithium Metal Batteries
Authors: Ye Xue , Fu Han , Zhang Yixiao , Wu Dazhuan , Zhong Yu , Wang Xiuli , Ouyang Xiaoping , Tu Jiangping 
Published: September 2024

AbstractSuccinonitrile (SCN) based plastic crystal electrolytes (SPCEs) have attracted much attention for lithium metal batteries due to their considerable ionic conductivity and thermal stability. Insufficient mechanical properties, weak reductive stability, and the presence of free SCN molecules can result in adverse interfacial reactions. Polymer introduction has been explored to address these challenges. However, the introduction of polymer affects the SCN state, leading to reduced ionic conductivity, potentially due to limited segmental motion of the polymer at room temperature. Herein, a cross‐linked network polymer strategy is proposed to modify the Li‐ion transport pathway in SPCE, aiming to significantly improve the ionic conductivity. The strong interaction between the polymer matrix and SCN enhances their mutual solubility, reduces the crystallinity of SCN, and forms a rapid conduction pathway (polymer—[SCN—Li+]). The ionic conductivity of SPCE increases to 1.28 mS cm−1, with the Li‐ion migration number (tLi+
) also rising to 0.7. Electrochemical performances in Li symmetrical, Li||LiFePO4 and Li||LiNi0.8Co0.1Mn0.1O2 cells show significant improvement at both room temperature and 0 °C. These findings suggest that designing polymer network structures in SPCEs holds promise for solid‐state lithium metal battery applications.
Potassium Diffusion in Mono‐ and Bi‐Crystalline SrTiO3 – Mechanisms and Activation Energies
Authors: Bernzen Janek , Fuchs Carmen , Jacob Timo , Ma Qian , Meyer Tobias , Jooss Christian , Weitzel Karl‐Michael 
Published: September 2024

AbstractThe diffusion of potassium in SrTiO3 (STO) single crystals is investigated as a function of temperature. Charge attachment induced transport experiments are employed inducing diffusion profiles in STO evolving with time. Potassium concentration profiles, characterized ex‐situ by ToF‐SIMS depth profiling, exhibited a bimodal shape indicating two different transport pathways. Two diffusion coefficients are obtained for the two profiles. Their temperature dependence is described using an Arrhenius approach, allowing two activation energies to be derived from the data set. Utilizing DFT+U, the ionic mobility of potassium along the crystal structure is simulated and activation energies are determined for every trajectory. The transport pathway with the larger diffusion coefficient is assigned to defect transport, most likely via Sr vacancies. The transport pathway exhibiting the lower diffusion coefficient is assigned to interstitial transport. In addition, the experiment is repeated on a bicrystalline STO sample to investigate the effect of a grain boundary on the ionic conductivity of the sample. As expected, the grain boundary represents an additional diffusion path for the potassium ions. The corresponding diffusion coefficient along the grain boundary is three orders of magnitude larger than that for bulk diffusion. Atomically resolved structural information in the grain boundary region is presented.
Copper‐Catalyzed Cross Coupling Reaction of Alkyl Bromides with (DMPU)2Zn(Rf)2 Reagent: A Method for the Synthesis of Perfluoroalkylated Compounds
Authors: Liu Bosheng , Jiang Xujuan , Song Yanshan , Liu Shiwen , Xiong Xiaodong , Zeng Xiaojun 
Published: September 2024

AbstractA method for the copper‐catalyzed cross‐coupling of alkyl bromides with a range of (DMPU)2Zn(Rf)2 reagents has been developed. This protocol tolerates multiple functional groups and provides broad access to aliphatic perfluoroalkylated compounds. The applicability of this procedure is demonstrated in the late‐stage functionalization of drug analogues.
Heterovalent State and Oxygen Vacancy Defect Structure‐Associated V/S Co‐Doped SnO2 for Catalytic Reduction of Organic and Cr6+ Pollutants in the Dark
Authors: Yang Baoqian , Wu Xinru , Su Zhengjie , Insua Benjamin Kunkadma , Zhang Pengkun , Kuo Dong‐Hau , Gao Lulu , Bao Xinde , Lu Dongfang , Lin Jinguo , Chen Xiaoyun 
Published: September 2024

AbstractV/S co‐doped SnO2 bimetal sulfur‐oxides catalysts labeled as (Sn,V)1‐x(S,O)2‐y or (SnVSO) with heterovalent state and oxygen vacancy defect are prepared via a green and facile method. The presence of SnVSO in the heterovalent states of Sn4+/Sn2+ and V5+/V4+ facilitates the rapid transfer of the electrons. It improves the electronic charge lifetime, accelerating the efficiency of the catalytic reduction of pollutants. The V/S co‐doped SnO2 regulates the bandgap energy structure. The hydrazine adjusts the heterovalent metal states to reduce Sn4+ to Sn2+ and V5+ to V4+. Also, it introduces oxygen vacancies to SnVSO to maintain the charge equilibrium and increase the active surface reactive sites, which enhance the catalytic activity. The SnVSO‐3 prepared with 0.4 mL hydrazine exhibits excellent catalytic activity, which wholly reduces 20 ppm of 100 mL methyl orange (MO), rhodamine B (RhB), methylene blue (MB), hexavalent chromium (Cr6+), and 4‐nitrophenol (4‐NP) within 6 min. In addition, the SnVSO‐3 also has good stability after repeated 6 runs with a reduction efficiency of 96.8%. Therefore, the V/S co‐doped SnO2 sulfur oxide catalysts have a promising potential for reducing Cr6+ and organic pollutants.
TRIM56 Modulates YBX1 Degradation to Ameliorate ZBP1‐Mediated Neuronal PANoptosis in Spinal Cord Injury
Authors: Lou Junsheng , Mao Yiting , Jiang Wu , Shen Honghao , Fan Yunpeng , Yu Qing , Zhou Conghui , Wei Ziyao , Zhou Kailiang , Jin Mengran , Wu Junsong 
Published: September 2024

AbstractSpinal cord injury (SCI) is a severe injury to the central nervous system, and its treatment is always a major medical challenge. Proinflammatory cell death is considered an important factor affecting neuroinflammation and the prognosis after injury. PANoptosis, a newly discovered type of proinflammatory cell death, regulates the activation of executioner molecules of apoptosis, pyroptosis and necroptosis through the PANoptosome, providing a new target for therapeutic intervention after SCI. However, its role and regulatory mechanism in SCI are not yet elucidated. Here, based on proteomic data, YBX1 expression is significantly increased in neurons after SCI. Guided by RIP‐seq, subsequent experiments reveal that YBX1 promotes ZBP1 expression by stabilizing the Zbp1 mRNA, thereby aggravating ZBP1‐mediated PANoptosis. Furthermore, the E3 ubiquitin ligase TRIM56 is identified as an endogenous inhibitor of YBX1 via molecular docking and IP/MS analysis. Mechanistically, TRIM56 bound to YBX1 and promoted its ubiquitination, thereby accelerating its degradation. Taken together, these findings reveal a novel function of YBX1 in regulating ZBP1‐mediated PANoptosis in the pathogenesis of SCI and verified that TRIM56 functions as an endogenous inhibitor to promote the ubiquitin‐proteasomal degradation of YBX1, providing new insights into SCI treatment strategies.
Breast Tumor Diagnosis Based on Molecular Learning Vector Quantization Neural Networks
Authors: Huang Chun , Shao Jiaying , Peng Baolei , Guo Qingshuang , Li Panlong , Sun Junwei , Wang Yanfeng 
Published: September 2024

AbstractDNA nanotechnology plays a crucial role in precise cancer medicine. Currently, molecular logic circuits are applied to detect tumor‐specific biomarkers and control the release of therapeutic drugs. However, these systems lack self‐learning capabilities for intelligent diagnostics in biological samples, and their data processing capabilities are limited. Here, a molecular learning vector quantization neural network (LVQNN) model based on DNA strand displacement (DSD) technology for breast tumor diagnosis is developed. Compared to previous work, the molecular LVQNN boasts powerful computing abilities, handling high‐dimensional data for intelligent cancer diagnosis. To verify the feasibility and versatility of the network, two distinct typical datasets are selected: one from a single source with cell morphology data from 569 cases, and a more extensive one spanning different populations and ages, with miRNA gene expression data from 1881 cases. By using the molecular LVQNN, diagnostic experiments are conducted on 50 and 120 public individuals from these two datasets, respectively, achieving accuracy rates of 94% and 97.5%. This study demonstrates that the LVQNN model exhibits significant advantages in breast cancer diagnosis and enhances diagnostic accuracy while introducing new approaches for intelligent cancer diagnosis, anticipated to bring significant breakthroughs and application prospects to precise cancer medicine.
Formation of Conjugated Polymer Monolayer Networks on Water Surface and Nonlinear Charge Transport
Authors: Ishizaki‐Betchaku Yuya , Hara Naoki , Matsuda Taikai , Matsui Jun , Seki Takahiro , Nagano Shusaku 
Published: September 2024

AbstractMaterial‐networked conduction paths provide nonlinear electronic properties, which are essential components of computing and physically mimic the brain. In this study, the formation of conjugated polymer monolayer networks and their nonlinear charge transport is demonstrated. Poly(3‐hexylthiophene) (P3HT) monolayer networks doped with 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4TCNQ) is fabricated using the co‐spread method with an amphiphilic liquid crystal molecule at the air–water interface. Atomic force microscopy and Ultraviolet–visible–near‐infrared absorption spectroscopy measurements reveal the network surface morphologies and doped electronic states. The correlation between the nonlinear electronic characteristics and network structures of the P3HT/F4TCNQ monolayer networks is further systematically investigated through current–voltage and voltage–time measurements for various doping levels, network densities, and numbers of transferred layers. The current–voltage characteristics of the P3HT/F4TCNQ monolayer network device with a simple two‐terminal structure exhibit nonlinear and ohmic conduction behavior, which depend strongly on the network density and geometric dimension (number of transferred layers). It is concluded that the nonlinear properties arise from the limited and unique network of 2D conduction passes. This study highlights the unique features of conducting polymer monolayer networks, paving the way for neuromorphic device applications including conjugated semiconducting polymer‐based material reservoirs with controllable nanostructures.
Recent Research on the Human Biology of Pastoralists
Authors: Campbell Benjamin 
Published: September 2024

ABSTRACTDespite encroachment by agricultural systems and globalization, pastoral nomads maintain a robust presence in terms of numbers and subsistence activity. At the same time, increasing concern about climate change has promoted awareness that increased climatic fluctuation may push pastoral population past their capacity for resilience. The response of pastoralists to climate change has important implications for our evolutionary past and our increasingly problematic future. Yet, pastoralists have received less explicit attention than foragers as populations under consistent selective constraints including limited caloric intake, high levels of habitual activity, and high disease burdens. Additional factors include exposure to cold and high temperatures, as well as high altitude. Over the last 20 or so years, the use of new techniques for measuring energetics, including actigraphs and doubly labeled water have built on existing noninvasive sample collection for hormones, immune markers and genes to provide a more detailed picture of the human biology of pastoral populations. Here I consider recent work on pastoralists from Siberia and northern Europe, Africa, Asia, and South America. I survey what is known about maternal milk composition and infant health, childhood growth, lactase persistence, and adult energy expenditure and lactase persistence to build a picture of the pastoralist biological response to environmental conditions, including heat, cold, and high altitude. Where available I include information about population history because of its importance for selection. I end by outlining the impact of milk consumption and climate over the human life cycle and make suggestions for further research.
Plasma miRNAs across the Alzheimer's disease continuum: Relationship to central biomarkers
Authors: Liu Shiwei , Park Tamina , Krüger Dennis M. , Pena‐Centeno Tonatiuh , Burkhardt Susanne , Schutz Anna‐Lena , Huang Yen‐Ning , Rosewood Thea , Chaudhuri Soumilee , Cho MinYoung , Risacher Shannon L. , Wan Yang , Shaw Leslie M. , Sananbenesi Farahnaz , Brodsky Alexander S. , Lin Honghuang , Krunic Andre , Blusztajn Jan Krzysztof , Saykin Andrew J. , Delalle Ivana , Fischer Andre , Nho Kwangsik ,   for the Alzheimer's Disease Neuroimaging Initiative
Published: September 2024

AbstractINTRODUCTIONMicroRNAs (miRNAs) play important roles in gene expression regulation and Alzheimer's disease (AD) pathogenesis.METHODSWe investigated the association between baseline plasma miRNAs and central AD biomarkers from the Alzheimer's Disease Neuroimaging Initiative (ADNI; N = 803): amyloid, tau, and neurodegeneration (A/T/N). Differentially expressed miRNAs and their targets were identified, followed by pathway enrichment analysis. Machine learning approaches were applied to investigate the role of miRNAs as blood biomarkers.RESULTSWe identified nine, two, and eight miRNAs significantly associated with A/T/N positivity, respectively. We identified 271 genes targeted by amyloid‐related miRNAs with estrogen signaling receptor–mediated signaling among the enriched pathways. Additionally, 220 genes targeted by neurodegeneration‐related miRNAs showed enrichment in pathways including the insulin growth factor 1 pathway. The classification performance of demographic information for A/T/N positivity was increased up to 9% with the inclusion of miRNAs.DISCUSSIONPlasma miRNAs were associated with central A/T/N biomarkers, highlighting their potential as blood biomarkers.Highlights
We performed association analysis of microRNAs (miRNAs) with amyloid/tau/neurodegeneration (A/T/N) biomarker positivity.
We identified dysregulated miRNAs for A/T/N biomarker positivity.
We identified Alzheimer's disease biomarker‐specific/common pathways related to miRNAs.
miRNAs improved the classification for A/T/N positivity by up to 9%.
Our study highlights the potential of miRNAs as blood biomarkers.
Development of a chronic compression spinal cord injury model in neonatal and adult rats
Authors: Ridlen Reggie , Marsters Victoria , Clarke Elizabeth , McGrath Kristine , Gorrie Catherine A. 
Published: September 2024

AbstractBackgroundSpinal cord injury presents a significant burden globally, with traumatic spinal cord injury being the predominant cause historically. However, nontraumatic spinal cord injury (NTSCI) is emerging as a significant contributor, particularly in developed nations, yet it remains poorly understood due to underreporting and misclassification. NTSCI, spanning various etiologies such as bony growths, vascular conditions, infections, neoplastic conditions, and immune disorders, poses unique challenges in diagnosis and treatment, often resulting in lifelong morbidity. This study addresses the lack of suitable animal models for NTSCI research, especially in neonatal animals.MethodsUtilizing a solid spacer approach, we developed a compression NTSCI model applicable to both neonatal and adult Sprague–Dawley rats.ResultsThrough anatomical measurements and in vivo experiments, we confirmed the feasibility and safety of the spacer insertion procedure and observed no acute off‐target effects.ConclusionThe versatility of this model lies in its adaptability to different ages of rats, offering a cost‐effective and reproducible means to induce graded injuries. Moreover, behavioral assessments demonstrated observable hindlimb function, validating the model's utility for studying functional outcomes. Although challenges persist, particularly in accounting for spinal column growth in neonatal animals, this model fills a crucial gap in pediatric NTSCI research. By providing a platform to investigate pathophysiological mechanisms and test potential treatments, it offers promising avenues for advancing our understanding and management of pediatric NTSCI.
Multi‐Scale Hierarchical Organic Photocatalytic Platform for Self‐Suspending Sacrificial Hydrogen Production from Seawater
Authors: Zhu Jingshuai , Dang Jie , Xiao Haoyuan , Wang Yuqi , Ding Lei , Zheng Jiaxin , Chen Jianming , Zhang Jianxiang , Wang Xungai , Xin John H. , Chen Shiguo , Wang Yuanfeng 
Published: September 2024

AbstractThe widespread application of photocatalysis for converting solar energy and seawater into hydrogen is generally hindered by limited catalyst activity and the lack of sustainable large‐scale platforms. Here, a multi‐scale hierarchical organic photocatalytic platform was developed, combining a photosensitive molecular heterojunction with a molecular‐scale gradient energy level alignment and micro‐nanoscale hierarchical pore structures. The ternary system facilitates efficient charge transfer and enhances photocatalytic activity compared to conventional donor‐acceptor pairs. Meanwhile, the super‐wetted hierarchical interfaces of the platform endow it with the ability to repeatedly capture light and self‐suspend below the water surface, which simultaneously improves the light utilization efficiency, and reduces the adverse effects of salt deposition. Under a Xe lamp illumination, the hydrogen evolution rate of this organic platform utilizing a sacrificial agent can reach 165.8 mmol h−1 m−2, exceeding that of mostly inorganic systems as reported. And upon constructing a scalable system, the platform produced 80.6 ml m−2 of hydrogen from seawater within five hours at noon. More importantly, the outcomes suggest an innovative multi‐scale approach that bridges disciplines, advancing the frontier of sustainable seawater hydrogen production driven by solar energy.
The Nature of Structural Defects in ZIF‐8 Revealed with 1H and 31P MAS NMR and X‐Ray Absorption Spectroscopy
Authors: Gabrienko Anton A. , Chaemchuen Somboon , Kou Zongkui , Ogiwara Naoki , Kitagawa Hiroshi , Khudozhitkov Alexander E. , Stepanov Alexander G. , Kolokolov Daniil I. , Verpoort Francis 
Published: September 2024

AbstractThe metal–organic frameworks (MOFs) attract interest as potential catalysts whose catalytic properties are driven by defects. Several methods have been proposed for the defects‐inducing synthesis of MOFs. However, the active species formed on the defective sites remain elusive and uncharacterized, as the spectroscopic fingerprints of these species are hidden by the regular structure signals. In this work, we have performed the synthesis of ZIF‐8 MOF with defect‐inducing procedures using fully deuterated 2‐methylimidazolate ligands to enhance the defective sites′ visibility. By combining 1H and 31P MAS NMR spectroscopy and X‐ray absorption spectroscopy, we have found evidence for the presence of different structural hydroxyl Zn−OH groups in the ZIF‐8 materials. It is demonstrated that the ZIF‐8 defect sites are represented by Zn−OH hydroxyl groups with the signals at 0.3 and −0.7 ppm in the 1H MAS NMR spectrum. These species are of basic nature and may be responsible for the catalytic activity of the ZIF‐8 material.
Low‐Temperature Flexibility of Chiral Organic Crystals with Highly Efficient Second‐Harmonic Generation
Authors: Lin Jiawei , Zhou Jianmin , Wang Zhihua , Li Liang , Li Maolin , Xu Jialiang , Wu Songgu , Naumov Panče , Gong Junbo 
Published: September 2024

AbstractFlexible crystals with unique mechanical properties have presented potential for applications in optoelectronics, soft robotics and sensors. However, there have been no reports of low‐temperature‐resistant flexible crystals with second‐order nonlinear optical properties (NLO). Here, we report flexible chiral Schiff‐base crystals capable of efficient second harmonic generation (SHG). Both enantiomers and the racemic form of these crystals are mechanically flexible in two directions at both room temperature and at 77 K, although their mechanical responses differ. The enantiomers display SHG with an intensity of up to 12 times that of potassium dihydrogenphosphate (KDP) when pumped at 980 nm, and they also have high laser‐induced damage thresholds (LDT). Even when bent, the crystals retain strong second harmonic generation, although with a different intensity distribution depending on the polarization, compared to when they are straight. This work describes the first instance of flexible organic single‐crystalline material with NLO properties and lays the foundation for the development of mechanically flexible organic NLO materials.
Exchange of CO2 with CO as Reactant Switches Selectivity in Photoreduction on Co−ZrO2 from C1–3 Paraffin to Small Olefins
Authors: Loumissi Tarik , Ishii Rento , Hara Keisuke , Oyumi Tomoki , Abe Ikki , Li Chongxu , Zhang Hongwei , Hirayama Rumiko , Niki Kaori , Itoi Takaomi , Izumi Yasuo 
Published: September 2024

AbstractPhotocatalytic reduction of CO2 into C2,3 hydrocarbons completes a C‐neutral cycle. The reaction pathways of photocatalytic generation of C2,3 paraffin and C2H4 from CO2 are mostly unclear. Herein, a Co0−ZrO2 photocatalyst converted CO2 into C1–3 paraffin, while selectively converting CO into C2H4 and C3H6 (6.0±0.6 μmol h−1 gcat−1, 70 mol %) only under UV/Visible light. The photocatalytic cycle was conducted under 13CO and H2, with subsequent evacuation and flushing with CO. This iterative process led to an increase in the population of C2H4 and C3H6 up to 61–87 mol %, attributed to the accumulation of CH2 species at the interface between Co0 nanoparticles and the ZrO2 surface. CO2 adsorbed onto the O vacancies of the ZrO2 surface, with resulting COH species undergoing hydrogenation on the Co0 surface to yield C1–3 paraffin using either H2 or H2O (g, l) as the reductant. In contrast, CO adsorbed on the Co0 surface, converted to HCOH species, and then split into CH and OH species at the Co and O vacancy sites on ZrO2, respectively. This comprehensive study elucidates intricate photocatalytic pathways governing the transformation of CO2 into paraffin and CO to olefins.