bluuebunny/crossref_metadata_2025_split huggingface dataset:
Operando Investigation of the Origin of C─C Coupling in Electrochemical CO2 Reduction Upon Releasing Bonding Strength, Structural Ordering in Pd─Cu Catalyst
Authors: Bagchi Debabrata , Riyaz Mohd , Dutta Nilutpal , Chawla Geetansh , R Churipard Sathyapal , Kumar Singh Ashutosh , C Peter Sebastian 
Published: August 2024

AbstractIt is widely established that the electroreduction of carbon dioxide on a copper surface yields a spectrum of alcohols and hydrocarbons. But the selectivity of Cu toward a certain product is extremely poor as it forms a variety of reduced products concurrently. Controlling selectivity and overall performance depends on the modification of the Cu site and local environment. This study depicts how the product selectivity can be switched from C1 to C2 and multicarbon products by systematic incorporation of secondary metal (Pd) into the Cu lattice. Upon releasing the structural ordering from intermetallic to alloy and then to bimetallic, a systematic enhancement on the formation of C2 products from CO2 has been observed. Real‐time in situ X‐ray absorption spectroscopy (XAS) study showed the potential dependent evolution of Pd─Cu and Cu─Cu bonds in different Pd‐Cu‐based catalysts. The detailed analysis of in situ IR and Raman also determined the adsorbed intermediate species and helped to identify the mechanism. Computational studies show the feasibility of multicarbon product formation on bimetallic catalysts compared to alloy and intermetallic catalysts. The current density and the activity of the CO2 electroreduction have been enhanced by the utilization of the flow cell in the gas diffusion electrode configuration.
In Situ Reconstructed Cu/β‐Co(OH)2 Tandem Catalyst for Enhanced Nitrate Electroreduction to Ammonia in Ampere‐Level
Authors: Qiao Lulu , Zhu Anquan , Liu Di , An Keyu , Feng Jinxian , Liu Chunfa , Ng Kar Wei , Pan Hui 
Published: August 2024

AbstractThe electrochemical nitrate reduction for green ammonia production is attracting increasing attention, where the catalysts are widely investigated by controlling the compositions or structures to achieve high performance. However, their reconstructions under reduction potentials are inevitable and uncontrollable, leading to uncertain performance, and a confused understanding of the mechanism. In this work, a strategy is proposed by controlling the pre‐catalyst's reconstruction chemistry toward electrochemical nitrate reduction reaction (e‐NO3RR) with superior activity and stability. To demonstrate the idea, a pre‐catalyst is fabricated with α‐Co(OH)2 and Cu(OH)2 (α‐Co(OH)2/Cu(OH)2), which is in situ reconstructed to a tandem catalyst with Cu and β‐Co(OH)2 (Cu/β‐Co(OH)2) under working potential. Cu/β‐Co(OH)2 achieves an optimal Faraday efficiency for ammonia of 97.7% with a yield rate of 3.9 mmol h−1 cm−2 at −0.5 V, outperforming other reported metal‐hydroxide catalysts. The experimental and theoretical results demonstrate that a tandem catalytic mechanism is responsible for the exceptional performance: 1) Cu functions as the donor of nitrite; and 2) β‐Co(OH)2 serves as active sites for generating active hydrogen and reducing nitrogen‐containing groups. This work highlights that the controllable reconstruction toward improved performance can be realized, and provides an insightful understanding of the mechanism, which is helpful for developing active and stable catalysts for various catalytic applications.
Prediction of ionic liquid surface tension via a generalized interpretable Structure‐Surface Tension Relationship model
Authors: Zhu Wenguang , Zhang Runqi , Liu Hai , Xin Leilei , Zhong Jianhui , Zhang Hongru , Qi Jianguang , Wang Yinglong , Zhu Zhaoyou 
Published: August 2024

AbstractIonic liquids' (ILs) surface tension, vital in liquid interface research, faces challenges in measurement methods—time‐consuming and labor‐intensive. The Structure‐Surface Tension Relationship (SSTR) is crucial for understanding the surface tension laws of ionic liquids, helping to predict surface tension and design ionic liquids that meet target requirements. In this study, SMILES string and group contribution methods were used to generate descriptors, and the random forest and multi‐layer perceptron (MLP) models were cross combined with the two descriptor generation methods to establish the SSTR model, providing a comprehensive framework for predicting the surface tension of ionic liquids. String‐MLP excels with high accuracy (R2 = 0.995, RMSE = 0.686, AARD% = 0.71%) for diverse ILs' surface tension values. Meanwhile, the Shapley Additive exPlanning (SHAP) method was used to test the impact of different features on model prediction, increasing the transparency and interpretability of the model.
Unraveling the relationship between microstructure of CMS membrane and gas transport property using molecular simulation
Authors: Hou Mengjie , Li Lin , Xu Ruisong , He Zilong , Lu Yunhua , Wang Tonghua , Jian Xigao 
Published: August 2024

AbstractCarbon molecular sieve (CMS) membranes are attractive for energy‐efficient gas separations. A challenge with the fabrication of a high‐performance CMS membrane is fine‐tuning its microstructure for precise and efficient separation. This necessitates a molecular‐scale analysis to understand its microstructure–performance relationship. Herein, molecular simulations were performed to unravel the relationships between four similar‐sized CMS matrices with different microstructural characteristics (e.g., chemical composition and micromorphology) and their gas transport properties. Results show that the disordered packing of carbon layers, leading to the formation of ultramicropore (2–7 Å), originates from stereoscopic sp3 hybridized carbon atoms rather than non‐carbon (oxygen) atoms. The size‐sieving ability of CMS depends positively on ultramicroporosity; the adsorption capacity is strengthened and then weakened with the increase of ultramicroporosity. Competitive effects are observed in binary‐mixture transport, and it is expected that the separation performance can be optimized by a reasonable distribution of ultramicropores combined with the affinity of oxygen‐containing species.
Impaired glymphatic function as a biomarker for subjective cognitive decline: An exploratory dual cohort study
Authors: Li Yuxia , Wang Luyao , Zhong Jiayi , Xu Huanyu , Han Ying ,   Alzheimer's Disease Neuroimaging Initiative, Zuo Chuantao , Jiang Jiehui 
Published: August 2024

AbstractBACKGROUNDSubjective cognitive decline (SCD) has been recognized as a potential risk stage for progression to Alzheimer's disease (AD), while glymphatic dysfunction is considered an important characteristic of AD. We hypothesize that glymphatic dysfunction occurs during the SCD stage, aiming to discover potential biomarkers for SCD.METHODSParticipants from two independent studies, Sino Longitudinal Study on Cognitive Decline (SILCODE, n = 654) and the Alzheimer's Disease Neuroimaging Initiative (ADNI, n = 650), representing different ethnicities and disease stages, were included to assess glymphatic function using diffusion tensor image analysis along the perivascular space (DTI‐ALPS).RESULTSAbnormal glymphatic function occurs during the SCD stage, with the ALPS index demonstrating excellent classification performance for SCD and normal controls (area under the receiver operating characteristic curve [AUC]SILCODE = 0.816, AUCADNI = 0.797). Lower ALPS index indicates higher risk of cognitive progression, which is negatively correlated with Subjective Cognitive Decline Questionnaire 9 scores and amyloid positron emission tomography burden.DISSCUSIONOur study suggests the ALPS index has the potential to serve as a biomarker for SCD.Highlights
Glymphatic function characterized by the analysis along the perivascular space (ALPS) index becomes abnormal in subjective cognitive decline (SCD), the earliest symptomatic manifestation and preclinical stage of Alzheimer's disease (AD).
The ALPS index demonstrates excellent classification performance for SCD and normal controls in the East Asian and Western cohorts.
Participants with a lower ALPS index show a higher risk of clinical progression.
The ALPS index is closely associated with serval cognitive scales and amyloid beta burden.
Deuteration and Tritiation of Pharmaceuticals by Non‐Directed Palladium‐Catalyzed C−H Activation in Heavy and Super‐Heavy Water
Authors: Teja Chitrala , Kolb Simon , Colonna Pierre , Grover Jagrit , Garcia‐Argote Sébastien , Lahiri Goutam Kumar , Pieters Grégory , Werz Daniel B. , Maiti Debabrata 
Published: August 2024

AbstractDeuterated and tritiated analogs of drugs are valuable compounds for pharmaceutical and medicinal chemistry. In this work, we present a novel hydrogen isotope exchange reaction of drugs using non‐directed homogeneous Pd‐catalysis. Aromatic C−H activation is achieved by a commercially available pyridine ligand. Using the most convenient and cheapest deuterium source, D2O, as the only solvent 39 pharmaceuticals were labelled with clean reaction profiles and high deuterium uptakes. Additionally, we describe the first application of non‐directed homogeneous Pd‐catalysis for H/T exchange on three different pharmaceuticals by using T2O as isotopic source, demonstrating the applicability to the synthesis of radiotracers.
Spatial‐coupled Ampere‐level Electrochemical Propylene Epoxidation over RuO2/Ti Hollow‐fiber Penetration Electrodes
Authors: Wang Jiangjiang , Dong Xiao , Feng Guanghui , Lu Xiaocheng , Wu Gangfeng , Li Guihua , Li Shoujie , Mao Jianing , Chen Aohui , Song Yanfang , Zeng Jianrong , Wei Wei , Chen Wei 
Published: August 2024

AbstractThe electrochemical propylene epoxidation reaction (PER) provides a promising route for ecofriendly propylene oxide (PO) production, instantly generating active halogen/oxygen species to alleviate chloride contamination inherent in traditional PER. However, the complex processes and unsatisfactory PO yield for current electrochemical PER falls short of meeting industrial application requirements. Herein, a spatial‐coupling strategy over RuO2/Ti hollow‐fiber penetration electrode (HPE) is adopted to facilitate efficient PO production, significantly improving PER performance to ampere level (achieving over 80 % PO faradaic efficiency and a maximum PO current density of 859 mA cm−2). The synergetic combination of the penetration effect of HPE and the spatial‐coupled reaction sequence, enables the realization of ampere‐level PO production with high specificity, exhibiting significant potentials for economically viable PER applications.
Working with adult families of origin: On the nature of rupture and repair
Authors: Cordukes Kate , U'Ren Greg , Katz Ella C. , McIntosh Jennifer E. 
Published: August 2024

AbstractIn this paper, we report on findings from a three‐part enquiry into the essence of working with families of origin where all members are adult. Findings, in conversational form, describe the nature of adult family ruptures encountered, pathways to repair and unique factors associated with the therapeutic encounter with adult families relative to those with still dependent children. In exploring emergent themes, we hoped to come to some understandings of the models and unique skill sets that characterise and enhance family therapy with adult families. We found that, unlike families with younger children, adult children are often the more motivated sub‐system and indeed the drivers of a referral for therapy. The therapeutic focus centred around legacy work from prior unresolved family traumas or disrupted developmental processes. Features of the therapeutic process included supporting new and more proportional narratives about ingrained wounds, together with redefinition of caregiving relationships and a future gaze towards becoming an independent yet connected family structure. We consider the therapist's posture in validating the adult child's experience, contextualising parent histories and clearing emotional barriers that block healthy giving and receiving of care. Key decision points in the therapist's work included how to balance the past context of the rupture with its current legacy, and the place of exoneration versus forgiveness in the progression towards secure individuation. Findings may help refine therapeutic methods in the application of systemic therapies with adult family forms, particularly on the intersection with the adult mental health system.
Self‐Calibration Temperature Sensing and Color Tunable Emission in a Bimetallic Lanthanide Metal–Organic Framework
Authors: Li Xiuzhen , Qi Xiangyue , Diao Xihui , Muhammad Yaseen , Chen Chao , Wang Hao , Qi Chuansong , Li Wei 
Published: August 2024

ABSTRACTTemperature in various scientific and industrial applications requires accurate detection and measurement. Herein, a range of novel isostructural lanthanide‐based metal–organic frameworks (Ln‐MOFs), [EuxTb2−x(3,5‐pdc)3(phen)2(H2O)2]n (x = 0, Tb‐MOF; x = 2, Eu‐MOF; x = 0.002, 0.010, 0.020, 0.040, 0.080, EuxTb2−x‐MOF), were solvothermally synthesized using 3,5‐pyridinedicarboxylic acid (3,5‐H2pdc) and 1,10‐phenanthroline (phen) as ligands. Based on binuclear second building units, Ln‐MOFs exhibited 2D layered structure with sql topology. The luminescent properties of series Ln‐MOFs show systematic tuning shifted from green to red by adjusting the ratio of Eu3+ to Tb3+. The temperature sensing experiments showed that Eu0.020Tb1.980‐MOF exhibited self‐calibration temperature response in a range of 293–413 K, achieving maximum relative sensitivity (Sr) 2.46%·K−1 at 413 K, outscoring many state‐of‐the‐art temperature sensors reported in literature. This study poses great promise of the newly designed Eu0.020Tb1.980‐MOF for the ultra‐sensitive temperature sensing in diverse and large‐scale applications.
Preparation and characterization of oxygen‐functionalized graphene‐doped polyvinylidene fluoride ultrafiltration membranes
Authors: Alemdar Sündüz , Pekel Bayramgil Nursel 
Published: August 2024

AbstractTo separate the oil/water mixtures, polyvinylidene fluoride (PVDF) nanofiber mats were produced using electrospinning. Additionally, PVDF films were made using the solvent evaporation method, and the effectiveness of their separation was evaluated against that of nanofiber mats. By choosing oxygen‐functionalized graphene (with HNO3) as a nano reinforcement, the hydrophobic properties of the PVDF materials made using both techniques were transformed into hydrophilic ones. It has been determined how the characteristics of the solution (viscosity, conductivity, molecular weight, surface tension, and contact angle) relate to the diameter of the nanofiber. Fourier transform infrared spectroscopy‐attenuated total reflection (FT‐IR/ATR), x‐rays diffraction (XRD), scanning electron microscope, thermogravimetric analyses (TGA)/DTG, and differential scanning calorimetric (DSC) have been used to study the chemical and crystal structures, morphology, and thermal behavior of PVDF materials. The addition of oxygen‐functionalized graphene was found to cause a peak in the PVDF composites' FT‐IR/ATR spectrum, roughly in the wavenumber 1400 cm−1, which was identified as the C‐OH bending vibration. Together with the shift in peak strengths, the lack of a discernible shift in the PVDF peak location in the XRD patterns indicates that the addition of oxygen‐functionalized graphene has caused a phase transition in the PVDF in the semi‐crystal structure. Surface hydrophobicity has also been measured using contact angle measurements. The addition of oxygen‐functionalized graphene has been seen to decrease the PVDF's contact angle, resulting in the development of a hydrophilic characteristic. These PVDF‐based materials' oil/water separation capabilities have also been evaluated. PVDF composite films were not as effective as PVDF nanofiber mats with oxygen‐functionalized graphene in the studies to separate the oil/water mixtures. The permeate flux value was determined to be 240 Lm−2 h−1, and the oil/water separation efficiency of nanofibers containing 10% (m/m) PVDF534000 combined with oxygen‐functional graphene was found to be 99%.
Data quality assurance practices in research data repositories—A systematic literature review. An Annual Review of Information Science and Technology (ARIST) paper
Authors: Stvilia Besiki , Pang Yuanying , Lee Dong Joon , Gunaydin Fatih 
Published: August 2024

AbstractData quality issues can significantly hinder research reproducibility, data sharing, and reuse. At the forefront of addressing data quality issues are research data repositories (RDRs). This study conducted a systematic analysis of data quality assurance (DQA) practices in RDRs, guided by activity theory and data quality literature, resulting in conceptualizing a data quality assurance model (DQAM) for RDRs. DQAM outlines a DQA process comprising evaluation, intervention, and communication activities and categorizes 17 quality dimensions into intrinsic and product‐level data quality. It also details specific improvement actions for data products and identifies the essential roles, skills, standards, and tools for DQA in RDRs. By comparing DQAM with existing DQA models, the study highlights its potential to improve these models by adding a specific DQA activity structure. The theoretical implication of the study is a systematic conceptualization of DQA work in RDRs that is grounded in a comprehensive analysis of the literature and offers a refined conceptualization of DQA integration into broader frameworks of RDR evaluation. In practice, DQAM can inform the design and development of DQA workflows and tools. As a future research direction, the study suggests applying and evaluating DQAM across various domains to validate and refine this model further.
Machine Learning Interatomic Potentials for Heterogeneous Catalysis
Authors: Tang Deqi , Ketkaew Rangsiman , Luber Sandra 
Published: August 2024

AbstractAtomistic modeling can provide valuable insights into the design of novel heterogeneous catalysts as needed nowadays in the areas of, e. g., chemistry, materials science, and biology. Classical force fields and ab initio calculations have been widely adopted in molecular simulations. However, these methods usually suffer from the drawbacks of either low accuracy or high cost. Recently, the development of machine learning interatomic potentials (MLIPs) has become more and more popular as they can tackle the problems in question and can deliver rather accurate results at significantly lower computational cost. In this review, the atomistic modeling of catalytic systems with the aid of MLIPs is discussed, showcasing recently developed MLIP models and selected applications for the modeling of heterogeneous catalytic systems. We also highlight the best practices and challenges for MLIPs and give an outlook for future works on MLIPs in the field of heterogeneous catalysis.
Evaporation of Binary Mixtures in a Pillow Plate Thermosiphon Reboiler
Authors: Jasch Katharina , Lu Yan , Scholl Stephan 
Published: August 2024

AbstractPillow plate heat exchangers show promising performance in extending the operating range of thermosiphon reboilers. Here, the evaporation of binary mixtures during natural circulation evaporation in a pillow plate apparatus was investigated. The experimental results show that the thermal performance is dominated by mixture effects and a component system‐dependent minimum is found. The model approach according to Bennett and Chen has proven to reliably estimate the product‐side heat transfer coefficient for pure substances and mixtures with a low boiling point distance. For wide‐boiling mixtures and low pressures the approach must be adjusted.
DOTAP Modified Formulations of Aminoacid Based Cationic Liposomes for Improved Gene Delivery and Cell Viability
Authors: Ravula Venkatesh , Muripiti Venkanna , Kumar Akash , Wang Li‐Fang , Kumar Vemula Praveen , Patri Srilakshmi V. 
Published: August 2024

AbstractThe liposomal systems proved remarkably useful for the delivery of genetic materials but enhancing their efficacy remains a significant challenge. While structural alterations could result in the discovery of more effective transfecting lipids, improving the efficacy of widely used lipid carriers is also crucial in order to compete with viral vectors for gene delivery. Herein, we developed formulations of commercially available lipid, 1,2‐dioleoyl‐3‐trimethylammonium‐propane (DOTAP) with synthetic amino acid based cationic lipids. Two cationic lipids were synthesized using amino acids, with either cystine (CTT) or arginine (AT) in the head group. These lipids were used to formulate co‐liposomal structures with different lipid compositions. The liposomal formulations were broadly categorised into two types: amino acid‐based liposomes without DOTAP (CTTD and ATD) and those with DOTAP (DtATD and DtCTTD). Optimized lipid‐DNA complexes of DOTAP‐incorporated formulations (DtATD and DtCTTD) exhibited enhanced efficacy in transfection compared to formulations lacking DOTAP as well as commercial formulations such as DOTAP:DOPE. Notably, DtCTTD displayed superior transfection capabilities in prostate cancer (PC3) and lung cancer (A549) cell lines when compared to the widely used commercial transfection reagent, Lipofectamine. Collectively, the findings from this study suggest that DOTAP‐incorporated formulations derived from amino acid‐based liposomes, hold promise as effective tools for improving transfection efficacy with reduced toxicity, offering potential advancements in gene delivery applications.
A Systematic Review and Narrative Synthesis Examining the Facilitators and Barriers of Psychological Intervention Delivery in Crisis Resolution Home Treatment Teams
Authors: Ahmed Haleemah , Bendall Caroline , Anwar Faiza , Al‐Janabi Mariam , Wood Lisa 
Published: August 2024

ABSTRACTBackgroundMental health crisis rates in the United Kingdom are on the rise. The emergence of community mental health models, such as Crisis Resolution Home Treatment Teams (CRHTTs), offers a vital pathway to provide intensive assessment and treatment to individuals in their homes, including psychological interventions. Previous qualitative literature has identified facilitators and barriers to the implementation of psychological interventions within CRHTT settings; however, a synthesis of this literature has not yet been conducted. To address this gap, a systematic review was undertaken with the aim of identifying the reported facilitators and barriers of implementing evidence‐based psychological interventions in CRHTTs.MethodA systematic review and narrative synthesis were conducted. Studies were included if they examined the implementation of evidence‐based psychological interventions in a CRHTT setting. The study population had to be 18 and over and could include healthcare professionals working in CRHTTs, service users of CRHTTs, or family and carers of CRHTT service users. Studies of any formal research methodology were included. Four databases were searched (MEDLINE, CINAHL Plus, Embase and PsycINFO), along with Google Scholar, to identify eligible studies.ResultsSix studies were identified, using mixed qualitative and quantitative methodologies, with the predominant focus being the exploration of stakeholder perspectives on care implementation within CRHTTs, encompassing aspects including but not restricted to psychological care implementation. The literature was deemed to be of moderate to high quality. Facilitators included adapting psychological therapies, prioritizing the therapeutic relationship, increasing psychological skills and training of CRHTT staff and psychologically informed CRHTT models. The barriers identified included a medical model bias within teams, resource constraints and elements pertaining to CRHTT services.ConclusionsFurther robust research in this area is imperative. We recommend that future research be implemented in the form of service evaluations and randomized controlled trials (RCTs) and that the principles of implementation science be used to assess and develop the evidence base for psychological intervention delivery in CRHTTs.