bluuebunny/crossref_metadata_2025_split huggingface dataset:
Adjusting Electronic Properties of Janus SHfAZ2 (A═Si,Ge; Z═N, P, As) via Strain Engineering and an Electric Field
Authors: Gao Zhen , He Yao , Xiong Kai 
Published: January 2024

AbstractIn this work, novel monolayers of 2D Janus SHfAZ2 (A═Si, Ge; Z═N, P, As) materials are introduced. These Janus structures are primarily investigated for their ability to exhibit adjustable electronic properties when subjected to biaxial strain and an applied electric field. At equilibrium, the four structures in the Janus SHfAZ2 monolayers all display indirect bandgap semiconductor properties, with the exception of the SHfGeN2 monolayer, which exhibits direct bandgap semiconductor properties. Under the influence of biaxial strain, the study observes that the electronic properties of all SHfAZ2 monolayers can be adjusted, transitioning from semiconductor to metallic properties when subjected to compressive strain. However, the SHfSiP2, SHfGeP2, and SHfGeAs2 monolayers show limited sensitivity to an applied electric field, with their electronic properties being modifiable solely under the influence of applied biaxial strain. In contrast, both the SHfSiAs2 and SHfGeN2 monolayers demonstrate the ability to modulate their electronic properties from semiconductors to metals when subjected to both biaxial strain and an applied electric field. Finally, the carrier mobility of these five structures is calculated. The outcomes of the research provide a solid theoretical foundation for the potential utilization of 2D Janus SHfAZ2 monolayers in electronic devices.
Stateful Logic Operation of Gated Silicon Diodes for In‐Memory Computing
Authors: Son Jaemin , Jeon Juhee , Cho Kyoungah , Kim Sangsig 
Published: January 2024

AbstractIn‐memory computing significantly reduces workload and energy cost of data access in the traditional von Neumann computing architecture. Using various memristors, stateful logic is developed to realize in‐memory computing. However, memristors have encountered critical issues in terms of device variation and reliability, and therefore, fundamental device solutions are required to realize practical stateful logic. In this study, NAND, NOR, and half‐adder stateful logic operations of gated silicon diodes with a p+–n–p–n+ structure are demonstrated to achieve in‐memory computing. Gated diodes have bistable, steep switching, and quasi‐nonvolatile memory characteristics, enabling reliable stateful logic operation. The uniformity of their device characteristics overcomes the inherent stochastic characteristics of memristors that are widely researched for stateful logic. The sequential multiread logic operation simplifies the complex state logic scheme. In particular, a nondestructive half‐adder operation can be executed in five sequential steps using six parallel diodes. Thus, the stateful logic of gated diodes can be a potential building block for in‐memory computing.
Asymmetric Atomic Tin Catalysts with Tailored p‐Orbital Electron Structure for Ultra‐Efficient Oxygen Reduction
Authors: Lin Xuanni , Zhang Xinqiang , Liu Dong , Shi Lei , Zhao Linjie , Long Yongde , Dai Liming 
Published: January 2024

AbstractAtomically dispersed transition metal–nitrogen–carbon (M–N–C) catalysts guide by the d‐band center theory have been extensively studied for oxygen reduction reaction (ORR) in various energy conversion and storage processes. However, asymmetric p‐block metal single‐atom catalysts (SACs) toward ORR have rarely been reported, and the origin of their catalytic activity is still unclear. Here, an asymmetric N, O coordinated Sn SAC is developed as an efficient ORR electrocatalyst. Remarkably, the optimized Sn SAC (e.g., Sn–N/O–C) exhibit outstanding ORR performance with a half‐wave potential of 0.910 V in alkaline media, outperforming most state‐of‐the‐art ORR catalysts. More importantly, the Sn–N/O–C possesses a long‐term durability in both alkaline and acidic electrolytes. Besides, Zn–air batteries based on the Sn–N/O–C cathode also show a higher energy density (254 mW cm‐2) than that of their reported M–N–C counterparts. Theoretical calculations suggest that the asymmetric N, O coordinated atomic Sn sites have a stronger binding interaction with O2 and better charge transfer ability compared with the symmetric SnN4 sites, thereby facilitating the ORR process. This work provides a nitrogen‐, oxygen‐coordinated engineering strategy for the rational design of highly active and durable carbon‐based catalysts with atomic p‐block metal sites for ORR and beyond.
Investigation of the impact of COVID‐19 on postoperative outcomes using a nationwide Japanese database of patients undergoing laparoscopic distal gastrectomy and low anterior resection for gastric cancer and rectal cancer
Authors: Akagi Tomonori , Endo Hideki , Inomata Masafumi , Shiroshita Hidefumi , Yamaguchi Shigeki , Eguchi Susumu , Wada Norihito , Kurokawa Yukinori , Seki Yosuke , Sakai Yoshiharu , Yamamoto Hiroyuki , Kakeji Yoshihiro , Kitagawa Yuko , Taketomi Akinobu , Mori Masaki 
Published: January 2024

AbstractBackgroundThe COVID‐19 outbreak made conventional medical care impossible, forcing changes in both healthcare providers and patients. In Japan, COVID‐19 infection began spreading in earnest in 2020 and exploded in 2021. There was concern that the medical impact of COVID‐19 in 2021 would differ from that in 2020. We aimed to clarify the impact of COVID‐19 on mortality and anastomotic leakage in laparoscopic surgery for gastric cancer and rectal cancer in Japan using the National Clinical Database (NCD).MethodsWe collected data from patients who underwent laparoscopic distal gastrectomy (LDG) and laparoscopic low anterior resection (LLAR) from January 2018 to December 2021 from the NCD, a web‐based surgical registration system in Japan. The number of surgical cases, monthly incidence of mortality and morbidity (anastomotic leakage), standardized mortality ratio (SMR), and standardized morbidity‐leakage ratio (SMLR [ratio of observed patients to expected patients calculated using the risk calculator established in the NCD]) were evaluated.ResultsThe numbers of LDG and LLAR cases continued to decline in the first year of the pandemic in 2020 and were as low in 2021 as in 2020. Although the numbers of robot‐assisted LDG and LLAR cases increased, the growth rate was lower than the rate of increase prior to the pandemic. Mortality and anastomotic leakage, two of the most important complications, as assessed by SMR and SMLR, did not worsen during the pandemic in comparison to the pre‐pandemic period.ConclusionsLaparoscopic surgeries were performed safely in Japan and were not affected by the COVID‐19 pandemic.
Selective electrooxidation glycerol to lactic acid coupled with hydrogen production over a cooperative BiOx/Au catalyst
Authors: Yan Yifan , Hao Pengjie , Fu Yu , Chen Wangsong , Shi Qiwei , Zhou Hua , Kong Xianggui , Li Zhenhua , Shao Mingfei , Duan Xue 
Published: January 2024

AbstractUtilizing sustainable electrocatalysis to upcycle glycerol (GLY; the by‐product of biodiesel) to lactic acid (LA; the key monomers for biodegradable polymer) is an efficient way to reduce the cost of biodiesel, which is also consistent with the waste‐to‐wealth principle. However, current research still suffers from issues of low LA selectivity (<80%), especially at high current density. Herein, we designed a cooperative catalyst by modifying BiOx nanolayers on gold nanoparticles (BiOx/Au), achieving high LA selectivity (82%) at high current density (226 mA cm−2 at 1.05 V vs. RHE), outperforming most of the reported works in the literature. We reveal that BiOx could promote the adsorption of the middle hydroxyl of GLY, which facilitates the formation of DHA and thus enables high LA selectivity. Moreover, the electron‐deficient Au in BiOx/Au is responsible for the enhanced current density, which is more beneficial to generate reactive oxygen species (OH*). To further reveal the application potential of this electrocatalytic strategy, we realized that the conversion of crude GLY extracted from cooking oil to LA coupled with H2 production using a membrane‐free flow electrolyzer, demonstrating a sustainable fashion to convert biodiesel waste into high value‐added product and H2 fuel.
Compliance with the 24‐h movement behaviors guidelines among urban and rural Brazilian preschoolers
Authors: Martins Clarice , Mota Jéssica , Goulart Natália , Silva Morgana , Silva Tamires , Carvalho Ferdinando , Mota Jorge , Bandeira Paulo Felipe , Lemos Luís 
Published: January 2024

AbstractBackgroundThe importance of movement behaviors for health is well‐known, although few studies have examined the compliance with movement guidelines in preschoolers from different living contexts. This study reported the compliance with the 24‐h movement behaviors guidelines among low‐income Brazilian preschoolers from rural and urban areas, according to age.MethodsA total of 453 preschoolers (n = 222 urban), aged between 3 and 5 years, provided physical activity (PA) data (Actigraph wGT3X). Sleep duration, and screen time were parent‐reported. Preschoolers were classified as compliant/non‐ compliant with the 24‐h movement guidelines, according to age. The association between prevalence of compliance with the recommendations and the children's living setting were estimated (SPSS; 27.0).ResultsPreschoolers were active (mean = 299.19 ± 76.42; and 369.76 ± 95.56 min/day in urban and rural areas, respectively), though moderate‐to‐vigorous physical activity (MVPA) time was below the 60 daily minutes recommended in both urban and rural settings (mean = 38.39 ± 21.36; and 47.32 ± 24.28, respectively). None of the urban children complied with the three recommendations simultaneously, while in the rural area, only 2.6% were compliant. Single movement behaviors compliances in the urban setting were 6.8%, 28.8% and 5.4% for PA, sleep, and screen time, respectively; while for rural settings were 16.5%, 21.2%, and 7.4%. Living in the rural area was related to the compliance with PA recommendation for the 5‐year‐old preschoolers.ConclusionIn both urban and rural Brazilian areas, very few preschoolers are compliant with the guidelines, and more than one third of the children do not comply with any of the recommendations. Strategies and programs to promote compliance with movement behaviors guidelines should consider children's living setting and their age groups.
Synthesis and Photophysical Evaluation of Dialkynyl‐N‐(het)arylpyrroles: Promising Key Compounds in Fluorescence Chemistry
Authors: Peglow Thiago J. , Nobre Patrick C. , Thomaz João Pedro S. S. C. , Vieira Marcelo M. , Junior Henrique C. S. , Dalberto Bianca T. , Schneider Paulo H. , Rodembusch Fabiano S. , Nascimento Vanessa 
Published: January 2024

AbstractIn this work, we present a series of chromophores based on dialkynyl‐N‐(het)arylpyrrole, featuring diverse combinations of donor‐acceptor moieties. The study explores the potential of fluorophores derived from (alkynyl)arylpyrroles, investigating the impact of the central core‘s nature with phenyl and pyridyl groups, along with various arylethynyl groups. Additionally, we assess these derivatives in the selective synthesis of non‐symmetrical ullazine derivatives with broad photophysical potential through photocatalysis. The precursors exhibit absorption maxima in the UVB region (~300 nm), while the model mono‐ullazine displays absorption maxima in the UVA region (~320 nm). Emission maxima for the precursors are observed between the UVA and violet regions, with the emission wavelength tailored by the substituents. In contrast, the mono‐ullazine fluoresces in the blue region. Remarkably, selected compounds exhibit an intricate photophysical behavior where a dual fluorescence emission with a large Stokes shift was present, which could not be clearly related to an intramolecular charge transfer (ICT) mechanism. Theoretical calculations support the experimental findings.
Behaviour support provision in Australia: A cross‐sectional survey of practitioners developing behaviour intervention plans
Authors: Kelly Glenn , Kremer Peter , Louise Kymberly , Fisher Alinka 
Published: January 2024

AbstractThere is currently a limited understanding of the characteristics of the workforce of behaviour support practitioners in Australia. A better understanding will help future considerations of training requirements, professional credentialling and associated professional regulation. A cross‐sectional online survey captured the demographic and work‐related characteristics of those who develop behaviour intervention plans for people with disability in Australia. The sample (n = 423) was primarily female (78 per cent), aged 26–45 years (57 per cent) and held a graduate (39 per cent) or postgraduate (53 per cent) degree. The largest single professional group was psychologists (28 per cent). The most common duration of experience was 1 year. Approximately half of the respondents were allied health practitioners either registered with the Australian Health Practitioner Regulation Agency or a member of the National Alliance of Self‐Regulating Health Professionals. The majority of practitioners had registered with the National Disability Insurance Scheme to provide behaviour support services (85 per cent). Both clients and services were concentrated in metropolitan regions, raising concerns regarding equity of access to behaviour support in remote communities, and among Aboriginal and Torres Strait Islanders. Given the vulnerability of many people with disabilities in receipt of behaviour support, ongoing policy and procedure work is needed to ensure professional credentialling and regulation of the workforce.
Cutting more than meals: Increasing severity of food insecurity is associated with the number and types of household financial strategies used to cope with inflation
Authors: Seivwright Ami , Kocar Sebastian , Visentin Denis , Kent Katherine 
Published: January 2024

AbstractFood insecurity is a prominent social determinant of health. There is evidence of increasing food insecurity in high‐income countries amid inflationary pressures. Yet, we know relatively little about the strategies that people employ to manage food insecurity nor how the severity of food insecurity affects the use of these strategies. Accordingly, this study of a nonprobability convenience online panel sample of 1284 adults in Tasmania assessed food insecurity and the strategies undertaken to manage rising costs of living. Structural equation modelling of 51 financial management actions revealed five strategies: reducing food quantity and quality, reducing housing and transport costs, drawing on assets, savings and credit, reducing insurance costs and reducing discretionary expenditure. Generalised linear regression modelling demonstrated that the use of coping strategies increased significantly with each categorical increase in food insecurity for each strategy except reducing insurance costs, in which increases became significant at moderate food insecurity. Overall, the results suggest that those experiencing food insecurity are also sacrificing in other areas, which is likely to have immediate and longer‐term effects on health, social and financial wellbeing. Opportunities to mitigate these consequences, including strengthening of social safety nets, nutrition programmes and structural investment to ensure universal access to food, are discussed.
Rhodium‐Catalyzed One‐Carbon Ring Expansion of Aziridines with Vinyl‐N‐triftosylhydrazones for the Synthesis of 2‐Vinyl Azetidines
Authors: Ning Yongquan , Chen Hongzhu , Ning Yongyue , Zhang Jin , Bi Xihe 
Published: January 2024

AbstractAzetidines, being four‐membered N‐heterocycles, possess significant potential in contemporary medicinal chemistry owing to their favorable pharmacokinetic properties. Regrettably, the incorporation of functionalized azetidines into pharmaceutical lead structures has been impeded by the absence of efficient synthetic methods for their synthesis. In this study, a Rh‐catalyzed one‐carbon ring expansion of aziridines with vinyl‐N‐triftosylhydrazones is presented, which facilitates the synthesis of high value‐added 2‐alkenyl azetidine products. This research represents the first example of ring expansion of aziridines enabled by vinyl carbenes. Additionally, a one‐pot two‐step protocol, initiated from cinnamaldehyde, was successfully achieved, offering a step‐economical and facile approach for the synthesis of these compounds. The pivotal aspect of this successful transformation lies in the in situ formation of an alkenyl aziridinium ylide intermediate. Experimental investigations, coupled with computational studies, suggest that a diradical pathway is involved in the reaction mechanism.
Review and Theoretical Analysis of Fluorinated Radicals in Direct CAr−H Functionalization of (Hetero)arenes
Authors: Fernandes Anthony J. , Giri Rahul , Houk Kendall N. , Katayev Dmitry 
Published: January 2024

AbstractWe highlight key contributions in the field of direct radical CAr− H (hetero)aromatic functionalization involving fluorinated radicals. A compilation of Functional Group Transfer Reagents and their diverse activation mechanisms leading to the release of radicals are discussed. The substrate scope for each radical is analyzed and classified into three categories according to the electronic properties of the substrates. Density functional theory computational analysis provides insights into the chemical reactivity of several fluorinated radicals through their electrophilicity and nucleophilicity parameters. Theoretical analysis of their reduction potentials also highlights the remarkable correlation between electrophilicity and oxidizing ability. It is also established that highly fluorinated radicals (e.g. ⋅OCF3) are capable of engaging in single‐electron transfer (SET) processes rather than radical addition, which is in good agreement with experimental literature data. A reactivity scale, based on activation barrier of addition of these radicals to benzene is also elaborated using the high accuracy DLPNO‐(U)CCSD(T) method.
Evolved Readers of 5‐Carboxylcytosine CpG Dyads Reveal a High Versatility of the Methyl‐CpG‐Binding Domain for Recognition of Noncanonical Epigenetic Marks
Authors: Kosel Brinja , Bigler Katrin , Buchmuller Benjamin C. , Acharyya Suchandra R. , Linser Rasmus , Summerer Daniel 
Published: January 2024

AbstractMammalian genomes are regulated by epigenetic cytosine (C) modifications in palindromic CpG dyads. Including canonical cytosine 5‐methylation (mC), a total of four different 5‐modifications can theoretically co‐exist in the two strands of a CpG, giving rise to a complex array of combinatorial marks with unique regulatory potentials. While tailored readers for individual marks could serve as versatile tools to study their functions, it has been unclear whether a natural protein scaffold would allow selective recognition of marks that vastly differ from canonical, symmetrically methylated CpGs. We conduct directed evolution experiments to generate readers of 5‐carboxylcytosine (caC) dyads based on the methyl‐CpG‐binding domain (MBD), the widely conserved natural reader of mC. Despite the stark steric and chemical differences to mC, we discover highly selective, low nanomolar binders of symmetric and asymmetric caC‐dyads. Together with mutational and modelling studies, our findings reveal a striking evolutionary flexibility of the MBD scaffold, allowing it to completely abandon its conserved mC recognition mode in favour of noncanonical dyad recognition, highlighting its potential for epigenetic reader design.
Development and Applications of D‐Amino Acid Derivatives‐based Metabolic Labeling of Bacterial Peptidoglycan
Authors: Zheng Yongfang , Zhu Xinyu , Jiang Mingyi , Cao Fangfang , You Qing , Chen Xiaoyuan 
Published: January 2024

AbstractPeptidoglycan, an essential component within the cell walls of virtually all bacteria, is composed of glycan strands linked by stem peptides that contain D‐amino acids. The peptidoglycan biosynthesis machinery exhibits high tolerance to various D‐amino acid derivatives. D‐amino acid derivatives with different functionalities can thus be specifically incorporated into and label the peptidoglycan of bacteria, but not the host mammalian cells. This metabolic labeling strategy is highly selective, highly biocompatible, and broadly applicable, which has been utilized in various fields. This review introduces the metabolic labeling strategies of peptidoglycan by using D‐amino acid derivatives, including one‐step and two‐step strategies. In addition, we emphasize the various applications of D‐amino acid derivative‐based metabolic labeling, including bacterial peptidoglycan visualization (existence, biosynthesis, and dynamics, etc.), bacterial visualization (including bacterial imaging and visualization of growth and division, metabolic activity, antibiotic susceptibility, etc.), pathogenic bacteria‐targeted diagnostics and treatment (positron emission tomography (PET) imaging, photodynamic therapy, photothermal therapy, gas therapy, immunotherapy, etc.), and live bacteria‐based therapy. Finally, a summary of this metabolic labeling and an outlook is provided.
Deciphering Structure‐Activity Relationship Towards CO2 Electroreduction over SnO2 by A Standard Research Paradigm
Authors: Guo Zhongyuan , Yu Yihong , Li Congcong , Campos dos Santos Egon , Wang Tianyi , Li Huihui , Xu Jiang , Liu Chuangwei , Li Hao 
Published: January 2024

AbstractAuthentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, the knowledge of the structure‐activity relationship can facilitate the design of efficient catalyst structures for specific reactivity requirements. However, understanding the relationship between a more realistic active surface and its performance is challenging due to the complicated interface microenvironment in electrocatalysis. Herein, we proposed a standard research paradigm to effectively decipher the structure‐activity relationship in electrocatalysis, which is exemplified in the CO2 electroreduction over SnO2. The proposed practice has aided in discovering authentic/resting surface states (Sn layer) of SnO2 accountable for the electrochemical CO2 reduction reaction (CO2RR) performance under electrocatalytic conditions, which then is corroborated in the subsequent CO2RR experiments over SnO2 with different morphologies (nanorods, nanoparticles, and nanosheets) in combination with in situ characterizations. This proposed methodology is further extended to the SnO electrocatalysts, providing helpful insights into catalytic structures. It is believed that our proposed standard research paradigm is also applicable to other electrocatalytic systems, in the meantime, decreases the discrepancy between theory and experiments, and accelerates the design of catalyst structures that achieve sustainable performance for energy conversion.