bluuebunny/crossref_metadata_2025_split huggingface dataset:
Low‐Coordinated Single‐Atom Catalysts Modulated by Metal Ionic Liquids for Efficient CO2 Electroreduction
Authors: Yuan Lei , Zeng Shaojuan , Li Guilin , Wang Yaofeng , Peng Kuilin , Feng Jiaqi , Zhang Xiangping , Zhang Suojiang 
Published: August 2023

AbstractModulating the coordination environment of single‐atom catalysts (SACs) is an attractive approach for maximizing the catalytic activity of single‐atom centers. Currently, the synthesis of low‐coordinated SACs is mainly confined to increasing the pyrolysis temperature (≥900 °C) to control C─N volatile fragments. Herein, a novel and universal strategy for the low‐coordinated SACs modulation is presented using transition metal (e.g., Ni, Co, Zn) ionic liquid precursors under relatively mild temperature of 600 °C, which regulates the L‐shell electronic structure and decreases nearly 50% electrophilic reactivity by ionization of 4‐position N atom, thereby orienting synthesis of the SACs with metal‐N3 centers. The Ni‐N3 SACs exhibit exceptional CO2 electroreduction performance of 99.7% CO Faraday efficiency with an ultra‐high CO partial current density of 467.55 mA·cm−2 as well as a CO production rate up to 10417.51 µmol·h−1·cm−2 in flow cell. The superior catalytic activity achieves over twofold increase compared with the Ni‐N4 SACs prepared by non‐metal ionic liquid precursors due to the lower free energy of the key intermediate *COOH and the stronger adsorption energy.
Charge Density Wave Order and Electronic Phase Transitions in a Dilute d‐Band Semiconductor
Authors: Chen Huandong , Zhao Boyang , Mutch Josh , Jung Gwan Yeong , Ren Guodong , Shabani Sara , Seewald Eric , Niu Shanyuan , Wu Jiangbin , Wang Nan , Surendran Mythili , Singh Shantanu , Luo Jiang , Ohtomo Sanae , Goh Gemma , Chakoumakos Bryan C. , Teat Simon J. , Melot Brent , Wang Han , Pasupathy Abhay N. , Mishra Rohan , Chu Jiun‐Haw , Ravichandran Jayakanth 
Published: August 2023

AbstractAs one of the most fundamental physical phenomena, charge density wave (CDW) order predominantly occurs in metallic systems such as quasi‐1D metals, doped cuprates, and transition metal dichalcogenides, where it is well understood in terms of Fermi surface nesting and electron–phonon coupling mechanisms. On the other hand, CDW phenomena in semiconducting systems, particularly at the low carrier concentration limit, are less common and feature intricate characteristics, which often necessitate the exploration of novel mechanisms, such as electron–hole coupling or Mott physics, to explain. In this study, an approach combining electrical transport, synchrotron X‐ray diffraction, and density‐functional theory calculations is used to investigate CDW order and a series of hysteretic phase transitions in a dilute d‐band semiconductor, BaTiS3. These experimental and theoretical findings suggest that the observed CDW order and phase transitions in BaTiS3 may be attributed to both electron–phonon coupling and non‐negligible electron–electron interactions in the system. This work highlights BaTiS3 as a unique platform to explore CDW physics and novel electronic phases in the dilute filling limit and opens new opportunities for developing novel electronic devices.
Fully Printed, High‐Temperature Micro‐Supercapacitor Arrays Enabled by a Hexagonal Boron Nitride Ionogel Electrolyte
Authors: Chaney Lindsay E. , Hyun Woo Jin , Khalaj Maryam , Hui Janan , Hersam Mark C. 
Published: August 2023

AbstractThe proliferation and miniaturization of portable electronics require energy‐storage devices that are simultaneously compact, flexible, and amenable to scalable manufacturing. In this work, mechanically flexible micro‐supercapacitor arrays are demonstrated via sequential high‐speed screen printing of conductive graphene electrodes and a high‐temperature hexagonal boron nitride (hBN) ionogel electrolyte. By combining the superlative dielectric properties of 2D hBN with the high ionic conductivity of ionic liquids, the resulting hBN ionogel electrolyte enables micro‐supercapacitors with exceptional areal capacitances that approach 1 mF cm−2. Unlike incumbent polymer‐based electrolytes, the high‐temperature stability of the hBN ionogel electrolyte implies that the printed micro‐supercapacitors can be operated at unprecedentedly high temperatures up to 180 °C. These elevated operating temperatures result in increased power densities that make these printed micro‐supercapacitors particularly promising for applications in harsh environments such as underground exploration, aviation, and electric vehicles. The combination of enhanced functionality in extreme conditions and high‐speed production via scalable additive manufacturing significantly broadens the technological phase space for on‐chip energy storage.
Programmable Dual‐Responsive Actuation of Single‐Hydrogel‐Based Bilayer Actuators by Photothermal and Skin Layer Effects with Graphene Oxides
Authors: Li Minghao , Bae Jinhye 
Published: August 2023

AbstractShape morphing of stimuli‐responsive composite hydrogels has received considerable attention in different research fields. Although various multilayer structures with dissimilar materials are studied to achieve shape morphing, combining swellable hydrogel layers with non‐swellable layers results in issues with interface adhesion and structural integrity. In this study, single‐hydrogel‐based bilayer actuators comprising poly(N‐isopropylacrylamide) (PNIPAM) matrices and graphene oxide (GO)–PNIPAM hinges are presented. Upon temperature rising, the PNIPAM hydrogel acts as the passive layer due to the formation of dense microstructures near the surface (i.e., the skin layer effect), whereas the GO‐PNIPAM hydrogel functions as the active layer, maintaining porous due to structural modification by the presence of GO. Under light exposure, the GO‐PNIPAM hinges experience selective heating due to the photothermal effect of GO. Consequently, the resulting bilayer structures exhibit programmable dual‐responsive 3D shape morphing. Additionally, the folding kinetics of these actuators can be adjusted based on the applied stimulus (temperature changes or light), as they are driven by different mechanisms, the skin layer, or photothermal effects, respectively. Furthermore, the hinge‐based bilayer structures demonstrate walking and steering locomotion by light exposure. This approach can lead to advances in soft robotics, biomimetic systems, and autonomous soft actuators in hydrogel‐based systems.
High‐Sensitive and Fast Speed UV Photodetector Based on HfSe2/InSe Heterostructure
Authors: Zhang Chengcheng , Zhang Shiji , Ding Jingzu , Wang Wenhui , Cao Zhangyu , Han Tao , Li Feng , Zhu Xiangde , Shan Lei , Long Mingsheng 
Published: August 2023

AbstractThe type‐II band‐aligned van der Waals (vdW) heterostructures are favorable for photocarrier separation and are often used for designing high‐performance photodetectors. Inspired by this, a metal‐mirror electrode enhanced HfSe2‐InSe vdW heterostructure photodetector is designed and demonstrated excitement performance in UV light detection. It is demonstrated the moderate bandgap heterostructure can be configured as a high‐performance UV photodetector with excellent light on/off ratio of 106, high photoresponsivity of 47.3 AW−1, competitive high specific detectivity of 3.2 × 1012 cmHz1/2W−1 and very low noise equivalent power of 2.8 × 10−16 WHz−1/2. Notably, the photoresponse speed of the device is very fast, with a rise time of 4.1 µs and a decay time of 5.4 µs. The results indicate that 2D HfSe2‐InSe vdW heterostructure possesses great potential applications in UV photodetection.
Road Narrow‐Inspired Strain Concentration to Wide‐Range‐Tunable Gauge Factor of Ionic Hydrogel Strain Sensor
Authors: Zhao Wenyu , Lin Zhuofan , Sun Zongtao , Zhu Zhihao , Lin Waner , Xu Yingtian , Peng Zhengchun , Sun Zhenglong , Wang Ziya 
Published: August 2023

AbstractThe application of stretchable strain sensors in human movement recognition, health monitoring, and soft robotics has attracted wide attention. Compared with traditional electronic conductors, stretchable ionic hydrogels are more attractive to organization‐like soft electronic devices yet suffer poor sensitivity due to limited ion conduction modulation caused by their intrinsic soft chain network. This paper proposes a strategy to modulate ion transport behavior by geometry‐induced strain concentration to adjust and improve the sensitivity of ionic hydrogel‐based strain sensors (IHSS). Inspired by the phenomenon of vehicles slowing down and changing lanes when the road narrows, the strain redistribution of ionic hydrogel is optimized by structural and mechanical parameters to produce a strain‐induced resistance boost. As a result, the gauge factor of the IHSS is continuously tunable from 1.31 to 9.21 in the strain range of 0–100%, which breaks through the theoretical limit of homogeneous strain‐distributed ionic hydrogels and ensures a linear electromechanical response simultaneously. Overall, this study offers a universal route to modulate the ion transport behavior of ionic hydrogels mechanically, resulting in a tunable sensitivity for IHSS to better serve different application scenarios, such as health monitoring and human–machine interface.
Large Improvement of Thermoelectric Performance by Magnetism in Co‐Based Full‐Heusler Alloys
Authors: Gui Zhigang , Wang Guiwen , Wang Honghui , Zhang Yuqing , Li Yanjun , Wen Xikai , Li Yikang , Peng Kunling , Zhou Xiaoyuan , Ying Jianjun , Chen Xianhui 
Published: August 2023

AbstractFull‐Heusler alloys (fHAs) exhibit high mechanical strength with earth‐abundant elements, but their metallic properties tend to display small electron diffusion thermopower, limiting potential applications as excellent thermoelectric (TE) materials. Here, it is demonstrated that the Co‐based fHAs Co2XAl (X= Ti, V, Nb) exhibit relatively high thermoelectric performance due to spin and charge coupling. Thermopower contributions from different magnetic mechanisms, including spin fluctuation and magnon drag are extracted. A significant contribution to thermopower from magnetism compared to that from electron diffusion is demonstrated. In Co2TiAl, the contribution to thermopower from spin fluctuation is higher than that from electron diffusion, resulting in an increment of 280 µW m−1 K−2in the power factor value. Interestingly, the thermopower contribution from magnon drag can reach up to ‐47 µV K−1, which is over 2400% larger than the electron diffusion thermopower. The power factor of Co2TiAl can reach 4000 µW m−1 K−2which is comparable to that of conventional semiconducting TE materials. Moreover, the corresponding figure of meritzTcan reach ≈0.1 at room temperature, which is significantly larger than that of traditional metallic materials. The work shows a promising unconventional way to create and optimize TE materials by introducing magnetism.
Fundamentals of Electrolyte Design for Wide‐Temperature Lithium Metal Batteries
Authors: Liu Qianqian , Wang Liguang 
Published: August 2023

AbstractLithium metal‐based batteries (LMBs) have garnered significant attention due to their exceptional energy density and lightweight characteristics. However, the electrochemical performance of LMBs often falls short, particularly in extreme temperature conditions. To address these challenges, the development of electrolytes capable of withstanding wide temperature ranges has emerged as a highly promising strategy for enhancing the operational capabilities of LMB across diverse weather conditions. This comprehensive review aims to explore the degradation mechanisms of wide‐temperature electrolytes, establishing a fundamental understanding of the failure mechanisms that impede LMB performance at harsh temperatures. Essential properties required for wide‐temperature electrolytes are elucidated, and the latest advancements in electrolyte technologies tailored specifically for all‐climate operations are comprehensively discussed. Particular emphasis is placed on the unique role of electrolyte solvation structure and interfacial properties across diverse weather conditions. This review offers valuable insights and proposes directions for the practical implementation of wide‐temperature electrolytes for LMBs, contributing significantly to the existing knowledge base while concurrently paving the way for developing robust LMBs capable of withstanding the rigors of diverse temperature environments.
Three‐Component Aza‐Diels‐Alder Reaction for the Syntheses of Tetrahydroisoquinoline Derivatives
Authors: Ngamnithiporn Aurapat , Chuentragool Padon , Ploypradith Poonsakdi , Ruchirawat Somsak 
Published: August 2023

AbstractReported herein is the development of a normal electron‐demand, three‐component aza‐Diels‐Alder reaction between sultines, aldehydes, and amines. In the presence of Cu(OTf)2 as a Lewis acid catalyst, the use of sultines as o‐quinodimethane precursors in conjunction with the in situ generation of imines enables the facile preparation of various polysubstituted tetrahydro‐isoquinoline derivatives from readily available substrates. The synthetic utility of these products was further explored through a number of product transformations, including the syntheses of tricyclic N‐heterocycles.
MIDA‐ and TIDA‐Boronates Stabilize α‐Radicals Through B−N Hyperconjugation
Authors: LaPorte Antonio J. , Feldner Jack E. , Spies Jan C. , Maher Tom J. , Burke Martin D. 
Published: August 2023

AbstractMultifunctional organoboron compounds increasingly enable the simple generation of complex, Csp3‐rich small molecules. The ability of boron‐containing functional groups to modify the reactivity of α‐radicals has also enabled a myriad of chemical reactions. Boronic esters with vacant p‐orbitals have a significant stabilizing effect on α‐radicals due to delocalization of spin density into the empty orbital. The effect of coordinatively saturated derivatives, such as N‐methyliminodiacetic acid (MIDA) boronates and counterparts, remains less clear. Herein, we demonstrate that coordinatively saturated MIDA and TIDA boronates stabilize secondary alkyl α‐radicals via σB‐N hyperconjugation in a manner that allows site‐selective C−H bromination. DFT calculated radical stabilization energies and spin density maps as well as LED NMR kinetic analysis of photochemical bromination rates of different boronic esters further these findings. This work clarifies that the α‐radical stabilizing effect of boronic esters does not only proceed via delocalization of radical character into vacant boron p‐orbitals, but that hyperconjugation of tetrahedral boron‐containing functional groups and their ligand electron delocalizing ability also play a critical role. These findings establish boron ligands as a useful dial for tuning reactivity at the α‐carbon.
Pushing the Upper Limit of Nucleophilicity Scales by Mesoionic N‐Heterocyclic Olefins
Authors: Eitzinger Andreas , Reitz Justus , Antoni Patrick W. , Mayr Herbert , Ofial Armin R. , Hansmann Max M. 
Published: August 2023

AbstractA series of mesoionic, 1,2,3‐triazole‐derived N‐heterocyclic olefins (mNHOs), which have an extraordinarily electron‐rich exocyclic CC‐double bond, was synthesized and spectroscopically characterized, in selected cases by X‐ray crystallography. The kinetics of their reactions with arylidene malonates, ArCH=C(CO2Et)2, which gave zwitterionic adducts, were investigated photometrically in THF at 20 °C. The resulting second‐order rate constants k2(20 °C) correlate linearly with the reported electrophilicity parameters E of the arylidene malonates (reference electrophiles), thus providing the nucleophile‐specific N and sN parameters of the mNHOs according to the correlation lg k2(20 °C)=sN(N+E). With 21<N<32, the mNHOs are much stronger nucleophiles than conventional NHOs. Some mNHOs even excel the reactivity of mono‐ and diacceptor‐substituted carbanions. It is exemplarily shown that the reactivity parameters thus obtained allow to calculate the rate constants for mNHO reactions with further Michael acceptors and predict the scope of reactions with other electrophilic reaction partners including carbon dioxide, which gives zwitterionic mNHO‐carboxylates. The nucleophilicity parameters N correlate linearly with a linear combination of the quantum‐chemically calculated methyl cation affinities and buried volumes of mNHOs, which offers a valuable tool to tailor the reactivities of strong carbon nucleophiles.
Design, synthesis, antimicrobial activity and molecular docking study of cationic bis‐benzimidazole‐silver(I) complexes
Authors: Üstün Elvan , Şahin Neslihan , Özdemir İlknur , Günal Selami , Gürbüz Nevin , Özdemir İsmail , Sémeril David 
Published: August 2023

AbstractTwo series of bis(1‐alkylbenzimidazole)silver(I) nitrate and bis(1‐alkyl‐5,6‐dimethylbenzimidazole)silver(I) nitrate complexes, in which the alkyl substituent is either an allyl, a 2‐methylallyl, an isopropyl or a 3‐methyloxetan‐3‐yl‐methyl chain, were synthesized and fully characterized. The eight N‐coordinated silver(I) complexes were screened for both antimicrobial activities against Gram‐negative (Escherichia coli, Pseudomonas aeruginosa, Klebsiella pneumoniae, and Acinetobacter baumannii) and Gram‐positive (Staphylococcus aureus, Staphylococcus aureus MRSA, and Enterococcus faecalis) bacteria and antifungal activities against Candida albicans and Candida glabrata strains. Moderate minimal inhibitory concentrations (MIC) of 0.087 μmol/mL were found when the Gram‐negative and Gram‐positive bacteria were treated with the silver complexes. Nevertheless, MIC values of 0.011 μmol/mL, twice lower than for the well‐known fluconazole, against the two fungi were measured. In addition, molecular docking was carried out with the structure of Escherichia coli DNA gyrase and CYP51 from the pathogen Candida glabrata with the eight organometallic complexes, and molecular reactivity descriptors were calculated with the density functional theory‐based calculation methods.
An analysis of the use of augmented reality and virtual reality as educational resources
Authors: de Moraes Rossetto Anubis G. , Martins Thauany C. , Silva Luís Augusto , Leithardt Daiana R. F. , Bermejo‐Gil Beatriz María , Leithardt Valderi R. Q. 
Published: August 2023

AbstractIn recent years, the utilization of augmented reality (AR) and virtual reality (VR) has emerged as a transformative approach in education, revolutionizing traditional teaching methods. This study seeks to explore the efficacy of AR and VR as pedagogical resources for enhancing the teaching of the solar system. The research process involved the development of an application comprising two modules, AR and VR, which were evaluated to assess their impact on the teaching process. Furthermore, a comparative study was conducted to evaluate the immersiveness, interactivity, and ease of use offered by these technologies. The findings demonstrate that both AR and VR demonstrate promise in supporting the teaching process, with the VR module garnering particularly positive evaluations. However, it is crucial to acknowledge existing barriers in underprivileged communities, where public schools face limited investments in technology infrastructure. These limitations hinder the widespread implementation of such immersive experiences and their potential to foster new knowledge acquisition.
Rare FGFR fusion genes in cervical cancer and transcriptome‐based subgrouping of patients with a poor prognosis
Authors: Hiranuma Kengo , Asami Yuka , Kato Mayumi Kobayashi , Murakami Naoya , Shimada Yoko , Matsuda Maiko , Yazaki Shu , Fujii Erisa , Sudo Kazuki , Kuno Ikumi , Komatsu Masaaki , Hamamoto Ryuji , Makinoshima Hideki , Matsumoto Koji , Ishikawa Mitsuya , Kohno Takashi , Terao Yasuhisa , Itakura Atsuo , Yoshida Hiroshi , Shiraishi Kouya , Kato Tomoyasu 
Published: August 2023

AbstractBackgroundAlthough cervical cancer is often characterized as preventable, its incidence continues to increase in low‐ and middle‐income countries, underscoring the need to develop novel therapeutics for this disease.This study assessed the distribution of fusion genes across cancer types and used an RNA‐based classification to divide cervical cancer patients with a poor prognosis into subgroups.Material and MethodsRNA sequencing of 116 patients with cervical cancer was conducted. Fusion genes were extracted using StarFusion program. To identify a high‐risk group for recurrence, 65 patients who received postoperative adjuvant therapy were subjected to non‐negative matrix factorization to identify differentially expressed genes between recurrent and nonrecurrent groups.ResultsWe identified three cases with FGFR3‐TACC3 and one with GOPC‐ROS1 fusion genes as potential targets. A search of publicly available data from cBioPortal (21,789 cases) and the Center for Cancer Genomics and Advanced Therapeutics (32,608 cases) showed that the FGFR3 fusion is present in 1.5% and 0.6% of patients with cervical cancer, respectively. The frequency of the FGFR3 fusion gene was higher in cervical cancer than in other cancers, regardless of ethnicity. Non‐negative matrix factorization identified that the patients were classified into four Basis groups. Pathway enrichment analysis identified more extracellular matrix kinetics dysregulation in Basis 3 and more immune system dysregulation in Basis 4 than in the good prognosis group. CIBERSORT analysis showed that the fraction of M1 macrophages was lower in the poor prognosis group than in the good prognosis group.ConclusionsThe distribution of FGFR fusion genes in patients with cervical cancer was determined by RNA‐based analysis and used to classify patients into clinically relevant subgroups.
Hybrid Catalysts for One‐pot Cascade Production of Gluconic Acid
Authors: Yang Ziyi , Wang Zhenfu , Dong Xiaoyan , Sun Yan 
Published: August 2023

AbstractGluconic acid is a valuable commodity in various industries such as pharmaceuticals, food, and construction. As the demand for gluconic acid grows, the development of its efficient and cost‐effective production methods has become a prominent research priority. Enzymatic synthesis has emerged as a promising approach for the production of gluconic acid due to its numerous advantages such as being eco‐friendly, highly efficient, and cost‐effective. Furthermore, the one‐pot catalytic method simplifies production equipment and operational steps. This concept review discusses the latest development in the field of multi‐enzymatic hybrid catalysts and chemo‐enzymatic hybrid catalysts for the one‐pot cascade catalytic production of gluconic acid. Perspectives for further research in this field are also provided to promote the application of multi‐enzyme complex cascade catalytic systems in extensive areas of organic synthesis.
Impact of Ultrasound Treatment Duration on Dihydrate Precursor Implying the Sesquihydrate Route
Authors: Palanychamy Prakas , Kong Leong Loong , Issabayeva Gulnaziya 
Published: August 2023

AbstractThe present invention relates to a technique for synthesizing vanadium phosphorus oxide (VPO) catalyst employing an ultrasonic treatment approach while assessing phase composition and hydrocarbon oxidation activity to a conventionally synthesized catalyst. The ultrasonic treatment approach has been shown to produce a catalyst with improved surface constitution and accelerated hydrocarbon conversion in 3 h, as opposed to the typically heating process, which takes 24 h. Product selectivity is influenced by the nature of the catalyst, with an integration consisting of (VO)2P2O7 (V4+) and VOPO4 (V5+) being optimal for high rate of conversion. A 39 % conversion rate and 89 % maleic anhydride selectivity were achieved under optimum reaction conditions.